I'm asking this question in the same spirit as this other question: Conjectures that have been disproved with extremely large counterexamples?.
What's a nice conjecture relating to finite groups, that first fails for a group of order $N$, with $N$ large? By "nice" I mean a conjecture with a balance between having a simple statement, one that first fails for a large $N$, and something that is not immediately obvious that it is going to fail.
An example might be the conjecture "if $G$ is a finite simple group, then it is the unique simple group of its order", which first fails for $N=20160$.
"Large" in this context is of course undefined, perhaps we'll say $N$ is "large" if the number of groups of order at most $N$ up to isomorphism is "large" in a more generic context. Perhaps I might suggest $N \geq 32$ as large, since $N= 32$ is the smallest number such that there are at least $100$ groups of order at most $N$. The bigger $N$ you can come up with, though, the better!
According to this answer by Chain Markov on the post I linked to, here are a few, ordered from smallest to largest (known) counterexample:
Automorphism group of a non-abelian group is non-abelian: counterexample at $N=64$.
All products of commutators of any finite group are commutators. Counterexample at $N=96$. (Also mentioned in a comment by Gerry Myerson on this question)
Automorphism groups of all finite groups not isomorphic to $\{e \}$ or $C_2$ have even order. Counterexample at $N=2187$ (automorphism group of said group has order $729$)
Moreto conjecture (very similar to the one I put in the body of the question): Let $S$ be a finite simple group and $p$ the largest prime divisor of $|S|$. If $G$ is a finite group with the same number of elements of order $p$ as $S$ and $|G| = |S|$, then $G \cong S$. Also fails at $N=20160$ with the simple groups of that order.
Any Leinster group has even order. Smallest known counterexample at $N=355433039577$.
Any nontrivial complete finite group has even order (a conjecture of S. Rose): smallest known counterexample at $N=788953370457$. (c.f. A341298 in the OEIS.)
Hughes conjecture: suppose $G$ is a finite group and $p$ is a prime number. Then $[G : \langle\{g \in G| g^p \neq e\}\rangle] \in \{1, p, |G|\}$. Smallest known counterexample at $N=142108547152020037174224853515625$.
Suppose $p$ is a prime. Then, any finite group $G$ with more than $\frac{p-1}{p^2}|G|$ elements of order $p$ has exponent $p$. Smallest known counterexample at $N=142108547152020037174224853515625$ (with $p=5$, same group as in the above one fails).
I'd be interested in any more people have.
Edit: Another answer of mine, kept separate, since it was not on Chain Markov's list.