Pope Paul VI appointed Leibold as the sixth archbishop of the Archdiocese of Cincinnati on July 23, 1969. He was installed on October 2, 1969. One historian has characterized Leibold as "both a warm-hearted, approachable pastor and a hard-worker." Leibold strengthened the Priests' Senate, the Pastoral Council, and the parish councils of the archdiocese. He also launched the archdiocese's sixth synod, Synod '71.
