A late 1959 Alvoturnos performance convinced Liberty Records talent scout Sonny "Confidential" Knight to recommend Yuro to label head Al Bennett, who immediately offered the singer a recording contract. But Yuro found Liberty's choice of material so frustrating that after months of recording lightweight demos ill-matched to her resonant, commanding voice, she crashed a 1961 label board meeting, vowing to Bennett and his colleagues to tear up her contract if they did not let her cut more appropriate material. She then performed an a cappella reading of the 1954 Roy Hamilton R&B hit "Hurt," so impressing the Liberty brass that in June 1961 Yuro entered the studio with producer Clyde Otis to record the song for posterity. A remarkably mature and assured debut record, "Hurt" peaked at number four on the Billboard pop charts that autumn, in addition to reaching number 22 on the R&B charts. No doubt viewers on both sides of the color line were shocked when Yuro's accompanying television appearances revealed this deeply emotional ballad was the work of a 20-year-old white woman less than five feet tall. Her follow-up single, a cover of the Charlie Chaplin composition "Smile," climbed to the number 42 spot in late 1961, and Liberty wrapped up the year with the release of "I Believe," a one-off effort pairing the singer with pop heartthrob Johnnie Ray.

Yuro spent early 1962 opening for Frank Sinatra on a brief tour of Australia. While the exposure no doubt boosted her profile, it was instrumental in crystallizing the growing public perception that she was more a cabaret performer than a soul singer, an image that was further established with her fourth single, a revival of "Let Me Call You Sweetheart" that went only as high as number 66 on the pop charts but cracked the easy listening Top 20. And despite its title, Yuro's sophomore LP, Soul!, proved to be a collection of standards, although she returned to her R&B roots with the superb Drifters homage "Count Everything." During sessions for her next effort, "What's a Matter Baby," producer Otis abruptly quit Liberty, and the masters were handed to his interim replacement, Phil Spector. The completed single bears all the hallmarks of the classic Spector sound, from its elegant string arrangement to its insistent rhythm to Yuro's righteously indignant vocal, and would prove her biggest hit since "Hurt," reaching number 12 on the pop charts and number 16 on its R&B counterpart. The team of Burt Bacharach and Hal David penned Yuro's next single, "The Love of a Boy," which climbed to number 44 in early 1963. Its follow-up, "Insult to Injury," went no higher than number 81 when it hit radio a few months later.

Following Ray Charles' successful embrace of country & western material, Yuro next covered Hank Cochran's "Make the World Go Away," scoring her last significant U.S. chart hit when the single reached number 24 on the pop charts and number eight on the easy listening chart. An album of country covers, also titled Make the World Go Away, yielded two more minor hits -- "Gotta Travel On" and "Permanently Lonely" -- and in the wake of 1964's "Should I Ever Love Again," Yuro cut ties with Liberty, signing to Mercury to release "If," which stalled at number 120. Her third Mercury effort, a rendition of Roy Hamilton's "You Can Have Him," was her only release on the label to crack the Hot 100, limping to the number 96 slot in early 1965. Teddy Randazzo authored Yuro's next release, the sublime "Get Out of My Life," and while the record was a commercial stiff, its flip side, "Can't Stop Running Away," would later resurface as a favorite of Britain's Northern soul community. Yuro returned to her Italian origins with the 1965 release "Ti Credo," recorded for entry in Italy's annual San Remo Festival. Her profile back home in the U.S. was by now virtually nonexistent, however, and subsequent Mercury releases including 1966's "Don't Keep Me Lonely Too Long" and the next year's bluesy cover of Johnny "Guitar" Watson's "Cuttin' In" went nowhere.

Yuro finally returned to Liberty in early 1968, traveling to Britain to cut her proposed comeback single, "Something Bad on My Mind." The finished product was her strongest release in some time, but went nowhere. Her breathtaking theme song to the Douglas Sirk film Interlude followed, and met a similarly grim fate (although Morrissey and Siouxie Sioux covered the tune a quarter century later); "It'll Never Be Over for Me" also stiffed, but also became a Northern soul perennial, with original copies changing hands for over 100 pounds a copy. A concert LP, Live at PJ's, was scheduled for release in the summer of 1969, but withdrawn just days prior to hitting retail. Yuro again left Liberty soon after, this time relocating to Las Vegas and starting a family. She performed only sporadically in the decade to follow, briefly resurfacing in 1975 on the short-lived Playboy label with "Southern Lady," which stalled at the number 108 spot. For Willie Mitchell's Frequency imprint, Yuro cut a stunning cover of Toussaint McCall's "Nothing Takes the Place of You" in 1979. A year later, she was diagnosed with throat cancer, but recovered to cut several LPs for the Dutch market as well as 1982's Timi Yuro Today, produced and financed by longtime friend Willie Nelson. Two years later she was forced to undergo a tracheotomy operation, effectively ending her singing career. She died March 30, 2004, at the age of 63.