Let $X_n \in \mathbb R^{n \times k}$ with $\mathop{\mathrm{rk}}\left(X_n\right) = k$.
Does $\lim_{n \to \infty} \left(X_n^\top X_n \right)^{-1} = 0_{\mathbb R^{k \times k}}$ hold if and only if $\lim_{n \to \infty}\mathop{\mathrm{tr}}\left[\left(X_n^\top X_n \right)^{-1} \right] = 0$?
I know that $\lim_{n \to \infty}\mathop{\mathrm{tr}}\left[\left(X_n^\top X_n \right)^{-1} \right] = 0$ implies that the positive square root of $\left(X_n^\top X_n \right)^{-1}$ vanishes, but I'm not sure if I'm on the right track with that.
You certainly know that if $A_n:=\left(X_n^\top X_n \right)^{-1}\to0_{\mathbb R^{k \times k}}$, then $\mathop{\mathrm{tr}}A_n\to0$ (by continuity of the trace map). Your question is then only about the converse.
Since each $A_n$ is symmetric positive, it can be written $B_n^\top B_n$ for some square matrix $B_n$, hence your question can be reworded:
You wrote in comment you "knew $\|B_n\|_{\text{Frobenius}}\to0\iff B_n\to0$, but didn't know that this implies $B_n^TB_n\to0$".
Well, it does: $$B_n\to0\implies B_n^TB_n\to0,$$ since transposition and matrix product (on fixed matrix spaces) are continuous.