After graduating from Perth Amboy High School, he entered Christ the Saviour Seminary in Johnstown, Pennsylvania, to study for the Holy Priesthood.
Upon graduation, he was ordained on January 11, 1959, by Bishop Orestes P. Chornock in Perth Amboy, N.J. His first pastorate was at Saints Peter and Paul Church in Windber, Pennsylvania, where he served until 1962.
Smisko studied at the Theological School of Halki on the island of Heybeliada in the Sea of Marmara near Istanbul for one year.
During his stay in the city, the young priest was assigned by the late Patriarch Athenagoras I to serve the spiritual needs of the large Slavic Orthodox community in the Galata section of Istanbul.
He also traveled extensively throughout Europe and the Middle East, visiting the sacred sites of the Holy Land and living for a time on Mount Athos, the ancient monastic center of the Orthodox Church.