From 1946-51, Fr Schmemann taught church history at St. Sergius. He was invited to join the faculty of Saint Vladimir’s Orthodox Theological Seminary, then in New York City, where he taught from 1951 onwards. When the seminary moved to its present campus in Crestwood, New York in 1962, Fr Schmemann assumed the post of dean, which he would hold until his death. He also served as adjunct professor at Columbia University, New York University, Union Theological Seminary and General Theological Seminary in New York. Much of his focus at St Vladimir's was on liturgical theology, which emphasizes the liturgical tradition of the Church as a major sign and expression of the Christian faith.

Fr Schmemann was accorded the title of protopresbyter, the highest honor that can be bestowed on a married Orthodox priest. He held honorary degrees from Butler University, General Theological Seminary, Lafayette College, Iona College, and Holy Cross Greek Orthodox School of Theology.

He was an Orthodox observer for the Second Vatican Council of the Roman Catholic Church from 1962 to 1965.

He was active in the establishment of the Orthodox Church in America and in its being granted autocephaly by the Russian Orthodox Church in 1970.

His sermons were broadcast in Russian on Radio Liberty for 30 years. He gained a broad following of listeners across the Soviet Union, including Aleksandr Solzhenitsyn, who became his friend after emigrating to the West.

Fr Schmemann published many books and articles. For the Life of the World, a popular volume on Christian faith as reflected in liturgy, has been translated into eleven languages. Originally prepared as study guide for the National Student Christian Federation in 1963, it even had an anonymous version published by the underground samizdat in the Soviet Union. The Eucharist was finished just before his death. This and several collections of his writings were published posthumously.

• Great Lent: Journey to Pascha (1969)
• For the Life of the World: Sacraments and Orthodoxy (1970)
• Liturgy and Life: Christian Development Through Liturgical Experience (1974)
• Of Water and the Spirit: A Liturgical Study of Baptism (1974)
• Introduction to Liturgical Theology (1975)
• The Historical Road of Eastern Orthodoxy (1977)
• Ultimate Questions: An Anthology of Modern Russian Religious Thought (1977)
• Church, World, Mission: Reflections on Orthodoxy in the West (1979)
• The Eucharist: Sacrament of the Kingdom (1988)
• Celebration of Faith: I Believe... (1991)
• Celebration of Faith: The Church Year (1994)
• Celebration of Faith: The Virgin Mary (1995)
• The Journals of Father Alexander Schmemann 1973-1983 (2000)