Performance wise...
1. Anthony Hopkins as Hannibal Lecter (The Silence of the Lambs)
2. Johnny Depp as Jack Sparrow (Pirates of the Caribbean: Curse of the Black Pearl)
3. Tom Cruise as Ethan Hunt (Mission Impossible III/Mission Impossible: Ghost Protocol)
Would be eager to see another movie from their respective franchises...
1. Ethan Hunt/Mission Impossible
2. Jack Sparrow/Pirates of the Caribbean
3. Hannibal Lecter
Mainly because, for me, the MI franchise thanks to Abrams and Bird feels like it can still surprise me, while I'm tired of Pirates especially after an attempt at something "new" with On Stranger Tides and frankly since Hannibal/Red Dragon didn't live up to The Silence of the Lambs, I doubt another one will be made or that Hopkins would ever return for.