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Talley was ordained as a priest on June 3, 1989 for the Archdiocese of Atlanta, and served as parochial vicar at St. Jude the Apostle Church in Atlanta until 1993. After earning his doctorate in Rome, he returned to Atlanta, serving as an officer of the archdiocesan tribunal and as director of vocations. Talley was named chancellor of the Archdiocese of Atlanta in October 1999.