Scorsese directed the actor in three films- 1980's "Raging Bull","Goodfellas" (1990), and "Casino" (1995).
Vincent passed away at the age of 78 on Wednesday after complications from open-heart surgery, reported Entertainment Weekly.
"Frank Vincent was someone I could count on. He was a natural who was at ease in front of the camera - on a set or on a stage. He made it look easy in all respects. He was genuine," Scorsese said in a statement.
"We worked together on three pictures, each time with his old partner Joe Pesci, and I always marvelled at his genius for improvisation.
"He was a hard-working actor, he understood the world we were portraying so well that he really didn't appear to be acting at all. I will always marvel at his artistry, and consider myself lucky to have had the chance to work with him and to know him," Scorsese added.
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