Film: Neon Demon and Midnight Run
Neon Demon was enjoyable for 2/3s as a stylistic exercise and by the end I wanted the film to end. Not what you want, IMO.
Midnight Run is fantastic. I loved the movie as a kid and it grows better with age. When DeNiro passes on and we need to reflect on 3 quintessential roles...I'll be in the minority, but I'll go with Mean Streets, Midnight Run, and Heat.
Obvious other candidates: Taxi Driver, Raging Bull, Goodfellas (overshadowed by Pesci), Silver Linings (his David O'Russell films), Cape Fear/Untouchables (crazy DeNiro), Meet the Parents (comedy DeNiro)
For me, it breaks down this way - there is Scorcese-DeNiro and you get to pick one performance. Taxi Driver or Raging Bull are the obvious ones, but I pick Mean Streets and I'll tell you why. Story goes - when studio execs first saw Mean Streets they thought Scorcese found DeNiro in an insane asylum. That does it for me.
Heat is the greatest film of the past 25 years and DeNiro out acts his rival, Pacino, in the quintessential coffee shop scene. This is DeNiro in his last "great" role, better than his Oscar winning Godfather 2 performance, IMO.
And lastly, comedy-DeNiro deserves a nod. He's been doing it now for 15 years and it basically encompasses the final act of his career. But who gives a shit about Meet the Parents and his roles in David O'Russell films are great, but really part of a ensemble and secondary. I go back to Midnight Run, a film where he's fucking hilarious and carries the movie. His scenes with Alonzo Mosley, the FBI agent are brilliant, including the genius physical comedy bit when he walks down the street with Mosley's FBI badge and stops and flashes it to no one in particular. The film also mixes in a great deal of emotion and the awkwardness of the scene between DeNiro and his daughter/ex-wife is painful to watch even today.