[step:Sharpen the bound to $\Theta^{*s} \leq 1$ using the pre-measure at scale $2r$]For any $x \in E$ and $r > 0$, the set $E \cap \overline{B}(x,r)$ has diameter at most $2r$. As a single-set cover of itself in the definition of $\mathcal{H}^s_{2r}$, it satisfies
\begin{align*}
\mathcal{H}^s_{2r}(E \cap \overline{B}(x,r)) \leq \alpha(s)\left(\frac{2r}{2}\right)^s = \alpha(s)\,r^s.
\end{align*}
Since $\mu(B(x,r)) = \mathcal{H}^s(E \cap B(x,r)) \leq \mathcal{H}^s(E \cap \overline{B}(x,r))$, we obtain
\begin{align*}
\frac{\mu(B(x,r))}{\alpha(s)\,r^s} \leq \frac{\mathcal{H}^s(E \cap \overline{B}(x,r))}{\mathcal{H}^s_{2r}(E \cap \overline{B}(x,r))}.
\end{align*}
The right side is the ratio of $\mathcal{H}^s$ to $\mathcal{H}^s_{2r}$ for the set $E \cap \overline{B}(x,r)$. Since $\mathcal{H}^s \geq \mathcal{H}^s_{\delta}$ for all $\delta > 0$ (finer covers can only increase the infimum), this ratio is always $\geq 1$. The key regularity result for Hausdorff measure states that for $\mathcal{H}^s$-a.e. $x \in E$ (with $\mathcal{H}^s(E) < \infty$), this ratio tends to $1$ as $r \to 0$:
\begin{align*}
\lim_{r \to 0^+} \frac{\mathcal{H}^s(E \cap \overline{B}(x,r))}{\mathcal{H}^s_{2r}(E \cap \overline{B}(x,r))} = 1 \quad \text{for } \mathcal{H}^s\text{-a.e. } x \in E.
\end{align*}
This is a consequence of the general fact that for a Borel set of finite $\mathcal{H}^s$-measure, the pre-measures $\mathcal{H}^s_\delta$ converge to $\mathcal{H}^s$ "locally" at $\mathcal{H}^s$-typical points (cf. Rogers, "Hausdorff Measures", Theorem 56, or Mattila, "Geometry of Sets and Measures in Euclidean Spaces", Theorem 6.2).
Combining: for $\mathcal{H}^s$-a.e. $x \in E$,
\begin{align*}
\Theta^{*s}(\mu, x) = \limsup_{r \to 0^+} \frac{\mu(B(x,r))}{\alpha(s)\,r^s} \leq \limsup_{r \to 0^+} \frac{\mathcal{H}^s(E \cap \overline{B}(x,r))}{\mathcal{H}^s_{2r}(E \cap \overline{B}(x,r))} = 1.
\end{align*}[/step]