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Marianne Faithfull, a British singer-songwriter and 1960s pop star who reinvented herself as a new-wave artist and smoky-voiced chanteuse, channeling her struggles with drug abuse and personal loss into songs of torment, anger, sorrow and resilience, died Jan. 30 in London. She was 78.

A spokesperson for Ms. Faithfull confirmed the death but did not provide a cause. Ms. Faithfull had battled years of health problems – including hepatitis C, breast cancer and an infection from a broken hip – before being hospitalized with covid in 2020. A year later, she told the New York Times that she was suffering from fatigue, memory problems and lung issues but was hoping to return to the stage.

A teen idol, film and stage performer, deadpan vocalist, ragged torch singer and cabaret queen, Ms. Faithfull was initially known as a poster child for rock-and-roll excess, a tabloid fixture who dated Rolling Stones frontman Mick Jagger before battling anorexia and heroin use. She attempted suicide in the early 1970s and spent several years on the streets of London, suffering persistent laryngitis that left her voice husky and raw.

“My career had been a fluke. … At best I was a curious anomaly in the mechanics of pop. As a performer I was only average,” she wrote in her 1994 autobiography, “Faithfull.”

Yet she made a triumphant comeback with the Grammy-nominated album “Broken English” (1979), embracing a darker, more intimate sound in songs such as Shel Silverstein’s “The Ballad of Lucy Jordan,” about a disillusioned suburban housewife. In recent years she drew renewed praise for albums including “Negative Capability” (2018), which combined new material with old standards and led a Rolling Stone reviewer to call her the “Grande Dame of Melancholy, the High Priestess of Dusky Rock.”

The album reaffirmed Ms. Faithfull’s reputation as a master interpreter of popular music, bringing new life over the years to songs by Dolly Parton, Randy Newman, Duke Ellington, Michel Legrand, Morrissey and Kurt Weill. She also worked with a varied cast of musicians, collaborating with artists including Metallica, Angelo Badalamenti, Nick Cave, PJ Harvey and David Bowie, with whom she performed “I Got You Babe” on a 1973 NBC variety show, dressed as a renegade nun in a backless habit.

Ms. Faithfull had turned toward music while studying at a Catholic convent school, performing in coffee houses and envisioning a future as a folk singer, if not an actor. But she said she was treated as “cheesecake” after Rolling Stones manager Andrew Loog Oldham spotted her in 1964, sitting on a heater at a London record-industry party at age 17 with blond hair, sparkling eyes and one of her boyfriend’s shirts tucked into her jeans.

“Who is she?” Oldham asked her date, according to Ms. Faithfull’s autobiography.

As Ms. Faithfull wrote, “That was that.”

Invited into the studio, she recorded the melancholy single “As Tears Go By,” later calling it “a commercial fantasy that pushes all the right buttons.” Written by Oldham, Jagger and Rolling Stones guitarist Keith Richards, it cracked the Top 10 in Britain and was recorded by the Stones in 1965.

The song thrust Ms. Faithfull and her quavering soprano into the acid-, booze- and grass-fueled center of the London music scene. She put out pop singles (“Come and Stay With Me”) and folk songs (“Blowin’ in the Wind” by Bob Dylan, whose advances she rejected), and in 1965 she simultaneously released her first two studio albums, the pop collection “Marianne Faithfull” and folksy “Come My Way.”

She also maintained a close association with the Stones. “I slept with three of them and then decided the lead singer was the best bet,” People magazine once quoted her as saying, explaining the origins of her four-year relationship with Jagger.

Ms. Faithfull performed at the group’s “Rock and Roll Circus” concert in 1968; contributed to the “whoo-whoo” backing vocals on their song “Sympathy for the Devil” (by some accounts it was inspired by the novel “The Master and Margarita,” which she gave to Jagger); and co-wrote “Sister Morphine,” a bluesy song about addiction that she released in 1969, two years before the Stones.

But her public image was transformed by a 1967 drug bust at Richards’s estate, which briefly landed him and Jagger in jail and led to Ms. Faithfull’s increasing villainization in the press. She was reportedly found by the police wearing nothing but a bearskin rug.

“They emerged with their reputations amplified as dangerous, glamorous outlaws. … I was destroyed by the very things that enhanced them,” she later wrote, according to Britain’s Observer newspaper.

In 1969, soon after Stones musician Brian Jones was dismissed from the band and found dead in his pool, Ms. Faithfull overdosed on barbiturates and entered a six-day coma. She awoke from her suicide attempt to see Jagger, who told her that she had seemed on the verge of death. In Ms. Faithfull’s telling, she replied, “Wild horses wouldn’t drag me away.”

By the time the Rolling Stones released “Wild Horses” in 1971, Ms. Faithfull and Jagger had split up. She had suffered a miscarriage, lost custody of a son from an early marriage and started using heroin, romanticizing the junkie lifestyle after reading William S. Burroughs’s novel “Naked Lunch.” “At that point,” she wrote in her autobiography, “I entered one of the outer levels of hell, and stayed there for years.”

She reemerged with “Broken English,” supported by musicians including keyboardist Steve Winwood and guitarist Barry Reynolds. The album included a propulsive cover of John Lennon’s “Working Class Hero”; a bouncy title song about the far-left German terrorist Baader–Meinhof Gang; and “Why D’ya Do It,” a sexually explicit punk-reggae number with lyrics from a Heathcote Williams poem.

“It isn’t anything we’ve heard before, from anyone,” rock critic Greil Marcus wrote in Rolling Stone. “As far as Faithfull goes, there’s a gutsiness here, a sense of craft and a disruptive intelligence that nothing in her old records remotely suggested. ‘Broken English’ is a kind of triumph: fifteen years after making her first single, Marianne Faithfull has made her first real album.”

“I gave myself permission to make a record that I’d wanted to make for a long time,” she later told Mojo magazine. “I thought I was going to die, that this was going to be my last chance to make a record. That is the thing about ‘Broken English,’ it’s this sense, this energy, that ‘ … before I die I’m going to show you … who I am.’ ”

Marianne Evelyn Gabriel Faithfull was born in London on Dec. 29, 1946.

Her father, Robert Glynn Faithfull, was a British intelligence officer and Italian literature instructor. Her mother, Austrian aristocrat Eva von Sacher-Masoch, was a onetime cabaret performer and relative of 19th-century author Leopold von Sacher-Masoch, whose name and writings inspired the term masochism.

Her parents met in Vienna during World War II and separated when she was 6. Her father moved to a utopian commune near Oxford, and her mother sent her to a Catholic boarding school in Reading.

At 18, she married artist John Dunbar, with whom she had a son, Nicholas. Their marriage ended in divorce, as did Ms. Faithfull’s later marriages to punk musician Ben Brierley, who worked on “Broken English,” and Giorgio Della Terza, a writer and actor.

Survivors include her son and three grandchildren.

At the height of her 1960s fame, Ms. Faithfull worked as an actor, appearing in movies such as “The Girl on a Motorcycle” (1968), an erotic film co-starring Alain Delon (“Your body is like a violin in a velvet case,” his character tells Ms. Faithfull’s), and director Tony Richardson’s 1969 adaptation of “Hamlet,” as Ophelia to Nicol Williamson’s scruffy Hamlet.

She later played God in the British sitcom “Absolutely Fabulous” and the devil in productions of “The Black Rider,” a musical collaboration involving Burroughs, Tom Waits and director Robert Wilson.

“Without showiness or actorly straining – but with a faint aura of rock ‘n’ roll sexual glamour still hovering around her – Ms. Faithfull explores a full and fascinating range of emotion,” Times movie critic A.O. Scott wrote of her performance in “Irina Palm” (2007) as a grandmother who becomes a prostitute.

Ms. Faithfull turned toward standards and cover songs after the release of “Broken English,” notably in the album “Strange Weather” (1987), her first full release since she was treated for heroin addiction. Her 21st solo album, “She Walks in Beauty” (2021), was completed after she was treated for covid-19 and featured readings of Romantic poems by Keats, Shelley and Wordsworth, set to music by Warren Ellis.

The album followed “Negative Capability,” her last with original material. “What can I do but pretend to be brave / And pretend to be strong when I’m not?” she sang on the closing track, “No Moon in Paris.” “There’s no moon, no moon in Paris tonight / And it’s lonely and that’s all I got.”

“It’s the most honest record I’ve ever made,” Ms. Faithfull told the Observer. “There are no hidden corners. … I’m afraid it’s open-heart surgery, darling.”