I also recommend Wages of Fear. Won't make my top 100 but very good. Le Corbeau is even better and is a smokey to make my list.
But the one film I would recommend over all others is Fellini's glorious La Dolce Vita, the story of a man who doesn't know what to do and doesn't know what he should feel. The movie grows on you tremendously, if you like it you will probably love it.