The Shining or Witches Of Eastwick?
Both stand out performances, and if you need reminding I recommend watching both films.
They belong in different genres which is why it's so difficult for me to pick out the better.
The Shining offered Mr Nicholson to demonstrate his descent in to madness, although he was barely holding on in the first place, while Witches Of Eastwick is a more darkly humorous outing that I believe has been under-rated.
Any other suggestions, that doesn't involve Tom Cruise.