When Charles W. Nibley was selected as the new Presiding Bishop of the church in 1907, he selected Smith as his second counselor. Smith was ordained a high priest and a bishop by Anthon H. Lund in December 1907. When first counselor Orrin Porter Miller died in 1918, Nibley made Smith his new first counselor. When Nibley was asked to join the First Presidency of the church in 1925, the new presiding bishop, Sylvester Q. Cannon, asked Smith to remain in the Presiding Bishopric as first counselor. Smith served in this capacity until April 6, 1938, when Cannon was released and became a member of the Quorum of the Twelve Apostles. As a member of the Presiding Bishopric, Smith was the head of LDS Hospital in Salt Lake City.
In 1908, Smith was made the first official president of the Mormon Tabernacle Choir. In this capacity, Smith's duties included managing the administrative, financial, and logistic details of the choir's increasing concert and tour schedule.[1][2] Smith was president of the choir until his release from the presiding bishopric in 1938.