On August 10, 1921, Curley was appointed the tenth archbishop of the Archdiocese of Baltimore by Pope Benedict XV. His installation took place on November 30, 1921. His arrival in his new city was described as "one of the greatest welcomes ever tendered a new citizen of Baltimore." During his tenure in Baltimore, Curley established 66 schools in 18 years, placing the importance of constructing schools over churches. In 1926, he declared, "I defy any system of grammar school education in the United States to prove itself superior to the system that is being maintained in the Archdiocese of Baltimore." He also established diocesan offices for Catholic Charities (1923) and for the Society for the Propagation of the Faith (1925). During the 1920s, Curley was a frequent critic of Irish President Eamon De Valera, comparing him to the Mexican revolutionary Pancho Villa. In March 1926, Curley criticized the expropriation of Catholic Church property by the Mexican Government and the expulsion of foreign priests and nuns:In order to preach the doctrine of Jesus Christ in Mexico, one must be a Mexican by birth. If the Savior of the world came back to Mexico, he would be exiled forthwith...because he is not a born Mexican.In 1931, Pope Pius XI appointed Curley as an assistant to the papal throne, becoming later a member of the College of Patriarchs and Bishops. The next year, Curley celebrated the mass at the end of the Eucharistic Conference in Dublin.
