Kill Bill vol1&2: Kill Bill has the perfect premise to become an amazing hack n slash game. Full of character, charm and style with the potential for great boss fights and set pieces. Also has an incredible soundtrack, would probably work well on the Metal Gear Rising engine. The Good the Bad and the Ugly: or perhaps the full dollars trilogy. Roaming the West as The Man With No Name would be an amazing experience, helping blow up the bridge to cease the battle for it, the fight through the town, escaping the prison and the final showdown would all be amazingly fun to play through. Another stellar soundtrack that could accompany it. Red Dead Redemption's engine would be a good starting point, but maybe even a more Call of Juarez styled game would work too. Sky Captain and the World of Tomorrow: Ok, the film isn't that great, the plot is watery at best and there wasn't an outstanding ost. But it was really, really stylish. Playing it out as maybe a side story to the film (or as the protagonist of the film, either works) you could explore the huge dieselpunk world, using the tech and visiting areas in the film. Would probably work really well with the engine Naughty Dog use for Uncharted. What films do you guys think would/should/could have really, really awesome tie-in video games?
V for Vendetta (2005 It would work well on the Assassin's Creed engine. You would play as V, a freedom fighter who gets his revenge on those who disfigured him. You would maneuver through the near-future U.K., stealthily taking care of your targets one by one (like the way you do in the Assassin's Creed series). The final mission would be igniting the revolution and exploding Parliament. There may even be side-missions where you play as Evey, with the player experiencing her transformation.
V for Vendetta would definitely be a good game, it could really work with a good moral system too. Do all good and the game plays out like the film, do a little bit of evil and it plays out more like the comic, that would be cool.
I Am Number Four - the book was mediocre and the movie was a little less than that, but it has a plot and premise that would make for a really fun video game. I've always been a fan of the whole 'people-with-powers' thing though, so that could just be my bias.