In Evans, Section 6.3, Theorem 4; we know that if $\Omega$ is a bounded region in $\mathbb{R}^n$ with smooth boundary (say), and $u\in H_0^1(\Omega)\cap H^2(\Omega)$ then we have the bound $\|u\|_{H^2}\le C(\|u\|_{L^2}+\|\Delta u\|_{L^2})$.
I've been agonizing over constructing a counterexample in $\Omega\subseteq \mathbb{R}^2$ to illustrate why no bound can hold when $u\in H^2(\Omega)$ alone. My first thought was to consider a sequence of harmonic functions whose gradients diverge in $L^2(\Omega)$, but I couldn't figure it out.
Your idea is good. Consider the sequence $u_n(x,y) = e^{nx}\sin ny$, in any fixed bounded domain $\Omega$. The functions are harmonic. Also, $$|\nabla u_n|^2 = n^2 e^{2nx}\sin^2 ny + n^2 e^{2nx}\cos^2 ny = n^2 e^{2nx}$$ which is substantially larger than $u_n^2 \le e^{2nx}$.