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At the age of thirteen, Ian wrote and sang her first hit single, "Society's Child (Baby I've Been Thinking)", about an interracial romance forbidden by a girl's mother and frowned upon by her peers and teachers: the girl ultimately decides to end the relationship, claiming the societal norms of the day have left her no other choice. Produced by George "Shadow" Morton and released three times between 1965 and 1967, "Society's Child" finally became a national hit upon its third release, after Leonard Bernstein featured it in a TV special titled Inside Pop: The Rock Revolution. The song's lyrical content was taboo for some radio stations, and they withdrew or banned it from their playlists accordingly; in her 2008 autobiography Society's Child, Ian recalls receiving hate mail and death threats as a response to the song, and mentions that a radio station in Atlanta that played it was burned down. In the summer of 1967, "Society's Child" reached #14 on the Billboard Hot 100, the single having sold 600,000 copies, and the album 350,000.

Ian relates on her website that, although the song was originally intended for Atlantic and the label paid for her recording session, the label subsequently returned the master to her and quietly refused to release it. Years later, Ian says, Atlantic's president at the time, Jerry Wexler, publicly apologized to her for this. The single and Ian's 1967 eponymous debut album were finally released on Verve Forecast; her album was also a hit, reaching #12. In 2001, "Society's Child" was inducted into the Grammy Hall of Fame, which honors recordings considered timeless and important to music history. Her early music was compiled on a double CD entitled Society's Child: The Verve Recordings in 1995.

Her most successful single in the United States was "At Seventeen", released in 1975, a bittersweet commentary on adolescent cruelty, the illusion of popularity, and teenage angst, as reflected upon from the perspective of a 24-year-old. "At Seventeen" was a smash, receiving tremendous acclaim from critics and record buyers alike — it charted at #3 on the Billboard Hot 100 and hit #1 on the Adult Contemporary chart. It won the 1975 Grammy Award for Best Pop Vocal Performance - Female beating out Linda Ronstadt, who was nominated for her Heart Like a Wheel album; Olivia Newton-John; and Helen Reddy. Ian performed "At Seventeen" as a musical guest on the debut of Saturday Night Live on October 11, 1975. The song's album, Between the Lines, was also a smash and hit #1 on Billboard's Album chart. It was quickly certified Gold and later earned a 'Platinum' certification for sales of over one million copies sold in the US. Another measure of her success is anecdotal: on Valentine's Day 1977, Ian received 461 Valentine cards, having indicated in the lyrics to "At Seventeen" that she never received any as a teenager.