Note that as $x \to 0$, we have $\tan(x) = x + \dfrac{x^3}{3} + O(x^5)$ (this is really a 2 line calculation). So,
\begin{align}
\tan^2(x) &= x^2 + \dfrac{2x^4}{3} + O(x^6)
\end{align}
Hence,
\begin{align}
\dfrac{\tan^2x - x^2}{x^2 \tan^2x} &= \dfrac{\frac{2x^4}{3} + O(x^6)}{x^4 + O(x^6)} \\
&= \dfrac{\frac{2}{3} + O(x^2)}{1 + O(x^2)},
\end{align}
where I divided top and bottom by $x^4$. Thus, if we take the limit $x \to 0$, the answer is $\dfrac{2}{3}$.
By the way, observe that it is no coincidence you had to differentiate $4$ times, because as you can see in the above derivation, the Taylor polynomials of the numerator and denominator begin at the $x^4$ term, so it is precisely the ratio of these coefficients which you're calculating if you use something like L'Hopital's rule.