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I have no idea if your critical percent can be reduced during combat, so I'm not actually 100% sure that 120% isn't completely redundant.
The real answer is no, but maybe.
I'm going to say there's no perks past 100%
Because of that, I don’t see a point to go past 100.
If it is "does 150% damage" that is totally valid and can in theory scale infinitely (which it does given the billions dmg numbers seen pre patch atleast).
However if it is "change to hit something/something to occur" it cannot go above 100% as that already is a guaranteed success. There is no such thing as "I succeeded more".
However the reason for "chance to hit" to go above 100% (game engine math wise) is if there are counter abilities that reduce your chance to hit, and the outcome would be the sum of those factors. I have no idea if this game has mechanics like that... I've not played enough yet.
And no, going over 100% is wasted.
Even going up to 100% is, since Critical Burn and Critical Moment are a thing.
These two alone can give you 75% crit chance and with the right Lumina combinations, you can make sure they are always active.
Got the numbers wrong. As I mentioned before, I haven't tested it myself.
https://www.reddit.com/r/expedition33/comments/1kjkshl/i_think_overcrits_are_a_thing/
EDIT: based on testing by EvilSod (see below), 300% crit vs 100% crit did not change his numbers
Alright, it's either a lie or the OP was severely mistaken.
With The One, Auto Death and Random Defence, I boosted Lune up to nearly 300% crit chance. Two casts of Hell, first dealt 464k, second dealt 475k (Warming Up).
Changed back to my regular pictos that don't influence damage and hit exactly 100% crit chance, the damage was identical.
So no, crit beyond 100% does nothing. Overcrit is not a thing.