It would be easy to just gesture vaguely at all of Sir Patrick Stewart's career. But your question was about better performances than in Trek, and I actually think he did an excellent Picard during the original TNG run. Not quite a hot take, I know.

However, for a double off-Trek billing, I suggest Green room (2015) where he plays against Anton Yelchin among others. It's a pretty taut little thriller about a punk band on the road that realise to their horror that their gig for the night is at a neonazi club out in the sticks. It goes downhill from there.