Lopes was born in Philadelphia, Pennsylvania, the daughter of Wanda Denise (nee Andino), a seamstress, and Ronald Lopes Sr., a US Army staff sergeant, of Portuguese background. She had a younger brother, Ronald Jr., and a younger sister, Raina Anitra (who professionally goes by Reigndrop). Lopes said her father was "very strict, very domineering" and that he treated the family like they were in "boot camp". He was a "talented musician" and played the harmonica, clarinet, piano, and saxophone.

At the age of 19, having heard of an open casting call for a new girl group through her then-boyfriend, Lopes moved to Atlanta to audition. Originally starting as a female trio called 2nd Nature, the group had been renamed TLC, derived from the first initials of its members at the time: Tionne, Lisa and Crystal. Things did not work out with Crystal Jones, and TLC's manager Perri "Pebbles" Reid brought in Damian Dame backup dancer Rozonda Thomas as a third member of the group. To preserve the band's original name, Rozonda needed a name starting with C, and so became Chilli, a name chosen by Lopes. Bandmate Tionne Watkins became T-Boz, derived from the first letter of her first name and "Boz" (slang for "boss"). Lopes was renamed "Left Eye" after a compliment from a man who once told her he was attracted to her because of her left eye. Lopes emphasized her nickname by wearing a pair of glasses with the left lens covered with a condom, in keeping with the group's promotion of safe sex, wearing a black stripe under her left eye, and eventually getting her left eyebrow pierced.  The group arrived on the music scene in 1992 with the album Ooooooohhh... On the TLC Tip. With four singles, it sold six million copies worldwide, leading to the group becoming a household name. Two years later CrazySexyCool was released, selling over 23 million copies worldwide, and cemented TLC as one of the biggest female groups of all time. TLC's third album, FanMail, was released in 1999 and sold over 14 million copies worldwide. Its title was a tribute to TLC's loyal fans and the sleeve contained the names of hundreds of them as a "thank you".  During the recording of FanMail, a public conflict began amongst the members of the group. In the May 1999 issue of Vibe magazine, Lopes said, "I've graduated from this era. I cannot stand 100 percent behind this TLC project and the music that is supposed to represent me." In response to Lopes' comments, Watkins and Thomas stated to Entertainment Weekly that Lopes "doesn't respect the whole group" and "Left Eye is only concerned with Left Eye." In response, Lopes sent a reply through Entertainment Weekly issuing a "challenge" to Watkins and Thomas to release solo albums and let the public decide who was the "greatest" member of TLC:  T-Boz and Chilli declined to take up the challenge, though Lopes always maintained it was a great idea. Things were heated between the ladies for some time, with Thomas speaking out against Lopes, calling her antics "selfish", "evil", and "heartless". TLC then addressed these fights by saying that they are very much like sisters that have their disagreements every now and then as Lisa stated, "It's deeper than a working relationship. We have feelings for each other, which is why we get so mad at each other. I usually say that you cannot hate someone unless you love them. So, we love each other. That's the problem."

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