Meet the Parents, the Prayer Scen

http://www.youtube.com/watch?v=Hrz7J--dWfM
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I'm finding it difficult to narrow it down his best, so I'll take the easy route and pick based on his most decorated performance, which is Raging Bull. Here is a full list of his awards
http://www.allmovie.com/cg/avg.dll?p=avg&sql;=2:17593~T3

Here is a great De Niro scene from The Deer Hunter
http://www.youtube.com/watch?v=lqakCa-MysE

/wait that Christopher Walkens best scene
Source(s):
http://www.allmovie.com/cg/avg.dll?p=avg&sql=2:17593~T3
http://www.mahalo.com/Robert%20De%20Niro

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Robert DeNiro is a great serious actor but I love him in comedies. I really don't know why but this scene from Analyze This is my favorite.

http://www.youtube.com/watch?v=_7cwHsN-fCc
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To me DeNiro's best movie is Goodfellas. It is one of my favorite films though so it is hard not to pick it. A pretty close tie would be Once Upon A Time In America. The cinematography and music in that film were off the charts, and the story was awesome too. Some great Deniro scenes in it as well. Loved it.

Although I think DeNiro is strong in both the above roles, however, I definitely think his best work was Raging Bull. A close second would be Meet the Parents just because Deniro the comedian is more engaging than the more intense dramatic version to me. I think my first film of his was Midnight Run when I was a kid, which if I recall was a comedy. Anyway, Meet the parents had some classic comedic acting moments, especially all the Mr. Jinks scenes.

Alas, since I cannot find my favorite Deniro scene from A Bronx Tail Online -- In the scene he and his son are listening to the Yankees game and cleaning up the bus after the last stop of the day. He gives his son this speech about the saddest thing in life being wasted talent. SUCH an awesome scene. I'll have to give a runner's up to Angel Heart though because for some reason I never seem to get the image out of my head of Mr. Deniro's long fingernails as he peels the hard boiled egg.
Source(s):
http://www.youtube.com/watch?v=AOb8sgghcrs

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