Following release of his gospel album for Mercury Records titled The King of the Gospel Singers, Little Richard met Mahalia Jackson, one of his childhood heroes. She was appearing in Los Angeles and he stopped her on the street to invite her to hear him sing at the Mount Maria Baptist Church. She attended and indicated that she was delighted with his singing, stating that "he was singing gospel songs the way they should be sung" and "he had that primitive beat and sound that came so naturally." Two of his gospel songs during this period hit the charts - "He's Not Just a Soldier" (1961) for Mercury, and "Crying In The Chapel" (1962) for Atlantic Records. He continued in the ministry but was experiencing marital problems and some difficulty living his ideal of a disciplined Christian life.
Although rock and roll sales were in a slump in America in 1962, Penniman's records were still selling well in England. British promoter Don Arden booked him for an October tour of the country, with The Beatles as an opening act. Penniman thought he was going to perform gospel music, but Arden had promoted the concert as a rock and roll show. On the first night of the tour he began performing gospel music, but gave in to the pressure and began performing his secular hits. He walked off to a standing ovation. The frenzied crowd reaction was to be repeated wherever he appeared
Penniman returned to Specialty Records in April 1963, recording one secular track. In mid-summer, around the time of Penniman's divorce, Don Arden began negotiating a second tour of England. Penniman did not disclose this to the church community because he was convinced that rock and roll was evil and still wanted to keep his options open in the ministry.
He toured England and Wales in October and November 1963, with Bo Diddley, The Everly Brothers and the then little-known Rolling Stones. Mick Jagger would later state, "I heard so much about the audience reaction, I thought there must be some exaggeration. But it was all true. He drove the whole house into a complete frenzy... I couldn't believe the power of Little Richard onstage. He was amazing." Near the end of the tour, he recorded a television show, The Little Richard Spectacular, with Sounds Incorporated as the backing band andThe Shirelles performing backing vocals, for Britain's largest independent television company at the time, Granada Network. After the show was first aired in May 1964, the Granada received over 60,000 letters from fans, which prompted the company to two repeat broadcasts of the show. Much of the footage was used for a TV special, highlighting the frenzy and excitement associated with rock and roll, that was seen all over the world.
Penniman recorded four more secular tracks for Specialty in April 1964. One of these recordings, "Bama Lama, Bama Loo" was released as a single and was a minor hit on the Billboard charts.
On March 1, 1964, he brought a fledgling Jimi Hendrix into his band, Hendrix began dressing and growing a mustache like Penniman's. He toured with Penniman and played on at least a dozen tracks for Vee Jay Records between the spring of 1964 and 1965. Three singles, including a cover of "Whole Lotta Shakin' Going On", would again hit the charts with moderate success.
Penniman continued to record and perform only secular music in the mid-60s, during which time he began drinking heavily. He has stated that he could have had more commercial success during this period, but southern preachers displeased with his backslide from the ministry pressured R&B radio stations throughout the southern U.S. not to play his music, while on the West Coast, particularly in Los Angeles following the Watts Riots, some black DJs were not playing his music because he was drawing both races to his concerts.
In 1966 and 1967, Penniman recorded two soul albums for Okeh Records, with his old friend from the mid-'50s, Larry Williams, as producer, and Johnny Guitar Watson on guitar. The first album produced the hit single, "Poor Dog." In August 1967, the second album, which was a collection of Okeh Club concert performances, returned Penniman to Billboard's Top 200 Albums chart for the first time in 10 years. Williams also acted as the musical director for Penniman's live performances used for the album, and Penniman's bookings during this period skyrocketed. This period also marked Penniman's return to a lifestyle of orgies and bisexuality, during which he also began dabbling incocaine.
With the emergence of the Black Power movement in the latter part of the decade, Penniman was invited to perform for strictly black crowds. He refused because he did not want to exclude any races from attending his shows. He remained a popular concert attraction, travelling extensively in the United States and Europe, as well as in Mexico and Canada, throughout the remainder of the decade.
In 1969, he was invited to perform at the Toronto Rock and Roll Revival. The event was filmed by director D.A. Pennebaker and also featuredChuck Berry, Bo Diddley, Jerry Lee Lewis and Gene Vincent.