[proofplan]
We construct the adjunction directly from the unit $\eta$ and counit $\varepsilon$. The map $\Phi_{c,d}$ sends a morphism $f: F c \to d$ to its adjunct $G(f)\circ \eta_c$, and the proposed inverse $\Psi_{c,d}$ sends $g: c \to Gd$ to $\varepsilon_d \circ F(g)$. The two triangle identities, together with naturality of $\eta$ and $\varepsilon$, show that these two assignments are inverse to each other. Finally, functoriality and naturality of $\eta$ verify naturality of the resulting hom-set bijection in both variables.
[/proofplan]
[step:Define the two transpose maps between the hom-sets]
Fix objects $c \in \mathcal C$ and $d \in \mathcal D$. Since $\mathcal C$ and $\mathcal D$ are locally small, the collections $\operatorname{Hom}_{\mathcal D}(F c,d)$ and $\operatorname{Hom}_{\mathcal C}(c,Gd)$ are sets.
Define
\begin{align*}
\Phi_{c,d}: \operatorname{Hom}_{\mathcal D}(F c,d) &\to \operatorname{Hom}_{\mathcal C}(c,Gd) \\
f &\mapsto G(f)\circ \eta_c,
\end{align*}
where $\eta_c: c \to G F c$ is the component of $\eta$ at $c$, and $G(f): G F c \to Gd$ is the image of $f:Fc \to d$ under $G$.
Define
\begin{align*}
\Psi_{c,d}: \operatorname{Hom}_{\mathcal C}(c,Gd) &\to \operatorname{Hom}_{\mathcal D}(Fc,d) \\
g &\mapsto \varepsilon_d \circ F(g),
\end{align*}
where $F(g): Fc \to F G d$ is the image of $g:c \to Gd$ under $F$, and $\varepsilon_d: F G d \to d$ is the component of $\varepsilon$ at $d$.
Both composites have the declared domains and codomains, so $\Phi_{c,d}$ and $\Psi_{c,d}$ are well-defined maps of sets.
[/step]
[step:Show that applying the transpose maps to $f:Fc \to d$ gives back $f$]
Let $f:Fc \to d$ be a morphism in $\mathcal D$. Then
\begin{align*}
\Psi_{c,d}(\Phi_{c,d}(f))
&= \Psi_{c,d}\bigl(G(f)\circ \eta_c\bigr) \\
&= \varepsilon_d \circ F\bigl(G(f)\circ \eta_c\bigr) \\
&= \varepsilon_d \circ F(G(f)) \circ F(\eta_c).
\end{align*}
By naturality of $\varepsilon:FG \Rightarrow \operatorname{id}_{\mathcal D}$ applied to the morphism $f:Fc \to d$, we have
\begin{align*}
f \circ \varepsilon_{Fc} = \varepsilon_d \circ F(G(f)).
\end{align*}
Substituting this equality gives
\begin{align*}
\Psi_{c,d}(\Phi_{c,d}(f))
&= f \circ \varepsilon_{Fc} \circ F(\eta_c).
\end{align*}
By the triangle identity at $c$,
\begin{align*}
\varepsilon_{Fc}\circ F(\eta_c)=\operatorname{id}_{Fc}.
\end{align*}
Therefore
\begin{align*}
\Psi_{c,d}(\Phi_{c,d}(f))
&= f \circ \operatorname{id}_{Fc} \\
&= f.
\end{align*}
[guided]
We start with a morphism $f:Fc \to d$ in $\mathcal D$ and follow it through the two proposed transpose operations. First $\Phi_{c,d}$ sends $f$ to
\begin{align*}
\Phi_{c,d}(f)=G(f)\circ \eta_c:c\to Gd.
\end{align*}
Applying $\Psi_{c,d}$ to this morphism gives
\begin{align*}
\Psi_{c,d}(\Phi_{c,d}(f))
&= \varepsilon_d \circ F\bigl(G(f)\circ \eta_c\bigr).
\end{align*}
Since $F$ is a functor, it preserves composition, so
\begin{align*}
F\bigl(G(f)\circ \eta_c\bigr)
=F(G(f))\circ F(\eta_c).
\end{align*}
Thus
\begin{align*}
\Psi_{c,d}(\Phi_{c,d}(f))
&= \varepsilon_d \circ F(G(f)) \circ F(\eta_c).
\end{align*}
The reason this expression simplifies is naturality of the counit. The natural transformation $\varepsilon:FG\Rightarrow \operatorname{id}_{\mathcal D}$ says that for every morphism $h:x\to y$ in $\mathcal D$,
\begin{align*}
h\circ \varepsilon_x=\varepsilon_y\circ F(G(h)).
\end{align*}
We apply this with $x=Fc$, $y=d$, and $h=f:Fc\to d$. This gives
\begin{align*}
f\circ \varepsilon_{Fc}=\varepsilon_d\circ F(G(f)).
\end{align*}
Substituting into the previous expression yields
\begin{align*}
\Psi_{c,d}(\Phi_{c,d}(f))
&= f\circ \varepsilon_{Fc}\circ F(\eta_c).
\end{align*}
Now the first triangle identity applies exactly to the remaining middle composite:
\begin{align*}
\varepsilon_{Fc}\circ F(\eta_c)=\operatorname{id}_{Fc}.
\end{align*}
Therefore
\begin{align*}
\Psi_{c,d}(\Phi_{c,d}(f))
&= f\circ \operatorname{id}_{Fc} \\
&= f.
\end{align*}
So $\Psi_{c,d}\circ \Phi_{c,d}$ is the identity map on $\operatorname{Hom}_{\mathcal D}(Fc,d)$.
[/guided]
[/step]
[step:Show that applying the transpose maps to $g:c \to Gd$ gives back $g$]
Let $g:c \to Gd$ be a morphism in $\mathcal C$. Then
\begin{align*}
\Phi_{c,d}(\Psi_{c,d}(g))
&= \Phi_{c,d}\bigl(\varepsilon_d \circ F(g)\bigr) \\
&= G\bigl(\varepsilon_d \circ F(g)\bigr)\circ \eta_c \\
&= G(\varepsilon_d)\circ G(F(g))\circ \eta_c.
\end{align*}
By naturality of $\eta:\operatorname{id}_{\mathcal C}\Rightarrow GF$ applied to the morphism $g:c\to Gd$, we have
\begin{align*}
G(F(g))\circ \eta_c=\eta_{Gd}\circ g.
\end{align*}
Substituting this equality gives
\begin{align*}
\Phi_{c,d}(\Psi_{c,d}(g))
&=G(\varepsilon_d)\circ \eta_{Gd}\circ g.
\end{align*}
By the triangle identity at $d$,
\begin{align*}
G(\varepsilon_d)\circ \eta_{Gd}=\operatorname{id}_{Gd}.
\end{align*}
Therefore
\begin{align*}
\Phi_{c,d}(\Psi_{c,d}(g))
&=\operatorname{id}_{Gd}\circ g \\
&=g.
\end{align*}
[guided]
Now we start with a morphism $g:c\to Gd$ in $\mathcal C$ and apply the two operations in the opposite order. The map $\Psi_{c,d}$ sends $g$ to
\begin{align*}
\Psi_{c,d}(g)=\varepsilon_d\circ F(g):Fc\to d.
\end{align*}
Applying $\Phi_{c,d}$ gives
\begin{align*}
\Phi_{c,d}(\Psi_{c,d}(g))
&=G\bigl(\varepsilon_d\circ F(g)\bigr)\circ \eta_c.
\end{align*}
Since $G$ is a functor, it preserves composition, so
\begin{align*}
G\bigl(\varepsilon_d\circ F(g)\bigr)
=G(\varepsilon_d)\circ G(F(g)).
\end{align*}
Hence
\begin{align*}
\Phi_{c,d}(\Psi_{c,d}(g))
&=G(\varepsilon_d)\circ G(F(g))\circ \eta_c.
\end{align*}
The expression $G(F(g))\circ \eta_c$ is simplified using naturality of the unit. The natural transformation $\eta:\operatorname{id}_{\mathcal C}\Rightarrow GF$ says that for every morphism $a:x\to y$ in $\mathcal C$,
\begin{align*}
G(F(a))\circ \eta_x=\eta_y\circ a.
\end{align*}
We apply this with $x=c$, $y=Gd$, and $a=g:c\to Gd$. This gives
\begin{align*}
G(F(g))\circ \eta_c=\eta_{Gd}\circ g.
\end{align*}
Substituting, we obtain
\begin{align*}
\Phi_{c,d}(\Psi_{c,d}(g))
&=G(\varepsilon_d)\circ \eta_{Gd}\circ g.
\end{align*}
Now the second triangle identity applies:
\begin{align*}
G(\varepsilon_d)\circ \eta_{Gd}=\operatorname{id}_{Gd}.
\end{align*}
Therefore
\begin{align*}
\Phi_{c,d}(\Psi_{c,d}(g))
&=\operatorname{id}_{Gd}\circ g \\
&=g.
\end{align*}
So $\Phi_{c,d}\circ \Psi_{c,d}$ is the identity map on $\operatorname{Hom}_{\mathcal C}(c,Gd)$.
[/guided]
[/step]
[step:Conclude that the transpose maps are bijections]
The previous two steps show that
\begin{align*}
\Psi_{c,d}\circ \Phi_{c,d}
&=\operatorname{id}_{\operatorname{Hom}_{\mathcal D}(Fc,d)}, \\
\Phi_{c,d}\circ \Psi_{c,d}
&=\operatorname{id}_{\operatorname{Hom}_{\mathcal C}(c,Gd)}.
\end{align*}
Hence $\Phi_{c,d}$ is a bijection with inverse $\Psi_{c,d}$ for every $c\in\mathcal C$ and $d\in\mathcal D$.
[/step]
[step:Verify naturality of the hom-set bijection in both variables]
Let $u:c'\to c$ be a morphism in $\mathcal C$, let $v:d\to d'$ be a morphism in $\mathcal D$, and let $f:Fc\to d$ be a morphism in $\mathcal D$. The induced morphism in $\operatorname{Hom}_{\mathcal D}(Fc',d')$ is
\begin{align*}
v\circ f\circ F(u):Fc'\to d'.
\end{align*}
We compute
\begin{align*}
\Phi_{c',d'}(v\circ f\circ F(u))
&=G(v\circ f\circ F(u))\circ \eta_{c'} \\
&=G(v)\circ G(f)\circ G(F(u))\circ \eta_{c'}.
\end{align*}
By naturality of $\eta$ applied to $u:c'\to c$,
\begin{align*}
G(F(u))\circ \eta_{c'}=\eta_c\circ u.
\end{align*}
Therefore
\begin{align*}
\Phi_{c',d'}(v\circ f\circ F(u))
&=G(v)\circ G(f)\circ \eta_c\circ u \\
&=G(v)\circ \Phi_{c,d}(f)\circ u.
\end{align*}
This is precisely the naturality condition for the family of bijections $\Phi_{c,d}$, contravariantly in $c$ and covariantly in $d$.
[guided]
The hom-set bijection must be compatible with changing both variables. Let $u:c'\to c$ be a morphism of $\mathcal C$ and let $v:d\to d'$ be a morphism of $\mathcal D$. A morphism $f:Fc\to d$ is transported on the $\mathcal D$-side by precomposition with $F(u):Fc'\to Fc$ and postcomposition with $v:d\to d'$, giving
\begin{align*}
v\circ f\circ F(u):Fc'\to d'.
\end{align*}
We apply $\Phi_{c',d'}$ to this transported morphism:
\begin{align*}
\Phi_{c',d'}(v\circ f\circ F(u))
&=G(v\circ f\circ F(u))\circ \eta_{c'}.
\end{align*}
Since $G$ is a functor, it preserves composition, so
\begin{align*}
G(v\circ f\circ F(u))
=G(v)\circ G(f)\circ G(F(u)).
\end{align*}
Thus
\begin{align*}
\Phi_{c',d'}(v\circ f\circ F(u))
&=G(v)\circ G(f)\circ G(F(u))\circ \eta_{c'}.
\end{align*}
The remaining expression involving $u$ is controlled by naturality of the unit. Applying naturality of $\eta:\operatorname{id}_{\mathcal C}\Rightarrow GF$ to the morphism $u:c'\to c$ gives
\begin{align*}
G(F(u))\circ \eta_{c'}=\eta_c\circ u.
\end{align*}
Substituting this identity gives
\begin{align*}
\Phi_{c',d'}(v\circ f\circ F(u))
&=G(v)\circ G(f)\circ \eta_c\circ u \\
&=G(v)\circ \Phi_{c,d}(f)\circ u.
\end{align*}
This equality says exactly that transposing after changing $f$ by $u$ and $v$ gives the same result as first transposing $f$ and then changing the resulting morphism $c\to Gd$ by precomposition with $u$ and postcomposition with $G(v)$. Hence the bijections are natural in both variables.
[/guided]
[/step]
[step:Identify the resulting adjunction]
For every $c\in\mathcal C$ and $d\in\mathcal D$, we have constructed a natural bijection
\begin{align*}
\operatorname{Hom}_{\mathcal D}(Fc,d)\cong \operatorname{Hom}_{\mathcal C}(c,Gd).
\end{align*}
By definition, this natural family of bijections is an adjunction with $F$ left adjoint to $G$. Therefore $F\dashv G$, with unit $\eta$ and counit $\varepsilon$ as stated.
[/step]