She never characterized herself as a jazz singer but dabbled in it at the company's request, and then was miscast in orchestra-laden pop songs with a nightclub feel. Hammond admitted later that Columbia had not adequately showcased her immense talents. Franklin's manager-husband, Ted White, urged her to seek another company when her Columbia contract expired, and Atlantic drew her away in 1967. Producer Jerry Wexler, responsible for her first sides for the label, took her to the Florence Alabama Music Emporium (FAME) in Muscle Shoals, Alabama, where Franklin was thrust into a capable group of musicians. There her vocal and piano abilities shined through and she was able to personally take charge of the arrangements. Unfortunately, Franklin only finished one song, "I Never Loved a Man (the Way I Love You)," before an altercation between a musician and White caused Franklin and her husband to dash out and disappear for a few weeks. Shortly thereafter, Wexler released the song to radio stations, who begged for more. Finally Franklin returned to New York and finished "Do Right Woman, Do Right Man," and later in 1967 released her first album for Atlantic, I Never Loved a Man (the Way I Love You). The late 1960s saw Franklin's career skyrocket with one hit single after another, including the million-selling "Baby I Love You," 1967, "Chain of Fools," 1967, "(Sweet Baby) Since You've Been Gone," 1968, "Think," 1968, "I Say a Little Prayer," 1968. Also in 1967, she recorded two of her trademark tunes, "(You Make Me Feel Like a) Natural Woman" and "Respect."

Franklin's rousing, thumping version of Otis Redding's "Respect" was released at an eventful moment in time, with civil rights, feminism, and sexual liberation all emerging into the forefront of American culture. Her fervent performance epitomized these movements and the record served as a theme song for social change. Franklin again represented an era, sadly, when she sang "Precious Lord" at the funeral of civil rights leader Reverend Dr. Martin Luther King, Jr., in 1968. King had been a close friend of Franklin's father. Franklin also sang the National Anthem at the Democratic Party's 1968 convention in Chicago, where riots ensued. In 1969, Franklin divorced Ted White and later began a romance with her road manager, Ken Cunningham. With him, she had her fourth child, Kecalf, whose name combines Cunningham's first name and Franklin's initials. Their six-year relationship ended in 1977.