He is also known for his film roles in Bang the Drum Slowly (1973), 1900 (1976), The King of Comedy (1982), Once Upon a Time in America (1984), Brazil (1985), The Mission (1986), Angel Heart (1987), The Untouchables (1987), Goodfellas (1990), This Boy's Life (1993), Mary Shelley's Frankenstein (1994), Heat (1995), Casino (1995), Jackie Brown (1997), Joker (2019), and The Irishman (2019).

Also known for his television roles, De Niro portrayed Bernie Madoff in the HBO film The Wizard of Lies (2017), earning a nomination for Primetime Emmy Award for Outstanding Lead Actor in a Limited Series or Movie.

[40] Pauline Kael of The New York Times was equally impressed by De Niro, writing he is "a bravura actor, and those who have registered him only as the grinning, tobacco-chewing dolt of that hunk of inept whimsey Bang the Drum Slowly will be unprepared for his volatile performance.

Set in gritty and morally bankrupt New York City following the Vietnam War, the film tells the story of Travis Bickle, a lonely taxi driver who descends into insanity.

Starring an ensemble cast, the film is set in the Emilia region of Italy, and tells the story of two men, the landowner Alfredo Berlinghieri (De Niro) and the peasant Olmo Dalcò (Gérard Depardieu), as they witness and participate in the political conflicts between fascism and communism in the first half of the twentieth century.

[55] Film critic Marie Brenner wrote, "it is a role that surpasses even his brilliant and daring portrayal of Vito Corleone in The Godfather Part II... his performance deserves to be compared with the very finest".

The drama, based on Oliver Sacks' 1973 book of the same title, tells the story of Dr. Malcolm Sayer (Robin Williams), who discovers benefits of the drug L-Dopa in 1969 and administers it to catatonic patients.

Owen Gleiberman of Entertainment Weekly gave the film a rating of "B−" and was critical of De Niro: "The actor who once got so far inside his roles that he just about detonated the screen – now plays characters who don't seem to have any inner life at all".

The feature received reasonable reviews and was lauded for the chemistry between De Niro and Murray; The Washington Post critic noted that their "real-life friendship spills over into this jittery, very funny look at the male bonding experience".

[112] De Niro starred in his directorial debut, A Bronx Tale (1993), a coming-of-age story about an Italian-American boy who is torn between the temptations of organized crime, racism in his community, and the values of his decent father.

A Bronx Tale premiered at the Toronto International Film Festival to a positive response; Marjorie Baumgarten of The Austin Chronicle wrote "De Niro's choices as a director all seem prudent and un-showy, designed to draw attention to the characters and the story rather than its technical assemblage and much-lauded star".

The film's themes revolve around greed, betrayal, wealth, status, and murder that occur between two mobsters, Sam "Ace" Rothstein (De Niro) and Nicky Santoro (Pesci), and a trophy wife (Stone) over a gambling empire.

[118] Roger Ebert was impressed with the lead performers' abilities to "inhabit their roles with unconscious assurance",[119] and The Globe and Mail's critic thought "De Niro does an extraordinarily subtle job of capturing the paradox [...] that lie at the heart of this picture".

In Heat, they represent a high postwar tradition for movie actors – the ones inspired by Marlon Brando, John Cassavetes and James Dean – who aren't afraid of emotion, who run right into the jaws of a scene to grab it.

The film's reception was generally unfavorable; William Arnold of the Seattle Post-Intelligencer took issue with the "in-your-face exaggeration", but he thought De Niro delivered "his usual edgy flair, [...] on the mean streets of his native Manhattan".

[148] Despite these failures, De Niro served as a producer for the critically acclaimed romantic-comedy About a Boy (2002), and appeared in 9/11 (2002), a CBS documentary about the September 11 attacks, told from the New York City fire department's point of view.

Writing for The Sydney Morning Herald, Sandra Hall noted its slow pace, stating "There's a potentially fascinating slice of American history here, but De Niro has carved it up with an excruciatingly dull knife".

[164] The following year, he starred in the police procedural thriller Righteous Kill opposite Al Pacino, both playing New York City detectives who investigate serial executions of criminals who escaped justice.

It was met with a mixed response; critic A. O. Scott complimented De Niro's ability for playing an estranged father (opposite Paul Dano), calling him "unpredictable and subtle", despite an uncertain plot.

[180][181] De Niro made his first appearance in a David O. Russell film, in the romantic comedy Silver Linings Playbook (2012), as the father of Pat Solatano (Bradley Cooper), who is released from a psychiatric hospital and moves back in with his parents to rebuild his life.

Co-starring Michael Douglas, Morgan Freeman, Kevin Kline and Mary Steenburgen, the film is about three retirees who travel to Las Vegas to have a bachelor party for their last remaining single friend.

The latter fared better with critics; Mark Olsen of the Los Angeles Times cordially remarked "De Niro brings a fresh, relaxed lightness to his performance, tinged with the gruff charm of Spencer Tracy".

[194] In 2017, De Niro starred as Bernie Madoff in Barry Levinson's HBO film The Wizard of Lies, a performance which earned him critical praise and a Primetime Emmy Award nomination for Outstanding Lead Actor in a Limited Series or Television Movie.

[195] In 2019, De Niro won acclaim for portraying Robert Mueller alongside Alec Baldwin's Donald Trump in various episodes of Saturday Night Live, earning him an Emmy nomination for Outstanding Guest Actor in a Comedy Series.

Released in October 2022, the ensemble includes Christian Bale, Margot Robbie, John David Washington, Michael Shannon, Mike Myers, Timothy Olyphant and Anya Taylor-Joy.

[209] In 2023, De Niro played William King Hale, a cattleman and perpetrator of the Osage Indian murders, in Killers of the Flower Moon, directed by Scorsese and adapted from the book of the same name by David Grann.

"[222] In 2009, he was announced as one of the Kennedy Center Honorees with the commemoration: "One of America's greatest cinematic actors, Robert De Niro has demonstrated a legendary commitment to his characters and has co-founded one of the world's major film festivals".

According to the FBI, similar devices were sent to high-profile politicians including Barack Obama, Hillary Clinton, Joe Biden, former Attorney General Eric Holder, and former CIA Director John Brennan.

[270][271] On April 19, 2021, De Niro's lawyer argued in a virtual divorce hearing presided by a Manhattan judge that he is "working at an unsustainable pace" in order "to support Hightower and pay off all his back taxes".

[295] Prolific in film since the 1970s, De Niro's most critically acclaimed films, according to the review aggregate site Rotten Tomatoes, include Bang the Drum Slowly (1973), Mean Streets (1973), The Godfather Part II (1974), Taxi Driver (1976), The Deer Hunter (1978), Raging Bull (1980), The King of Comedy (1983), Once Upon a Time in America (1984), Brazil (1985), The Mission (1986), Midnight Run (1988), Goodfellas (1990), Casino (1995), Heat (1995), Meet the Parents (2000), Silver Linings Playbook (2012), The Irishman (2019), and Killers of the Flower Moon (2023).