He also served as a professor of canon law, liturgy, spirituality, and ecclesiastical history, and the Dean of Theology at the Scholasticate.

Villeneuve founded the School of Superior Ecclesiastical Studies, where he was made titular professor of canon law, in 1928.

"[1] The Canadian primate was one of the cardinal electors who participated in the 1939 papal conclave, at which he himself was considered papabile,[2][3] that selected Pope Pius XII.

Villeneuve was stricken by a heart attack on July 7, 1946, while returning from Île-à-la-Crosse, where he had taken part in the celebrations for the centennial of his order.

On January 24, Cardinal James Charles McGuigan celebrated his funeral Mass, at which, according to Villeneuve's will, there was no eulogy but only Gregorian music.

[citation needed] During the autumn of 1944, he visited the Canadian military that were stationed in Great Britain, Italy, Belgium, and the Netherlands.