As Waterville's French-immigrant population increased, so did the desire of those French speaking Catholics, living in the neighborhood known as "The Plains", for a church building closer to their section of the city. In 1910, the newly formed parish of Notre Dame du Perpetual Secours (Ou r Lady of Perpetual Help) was separated from St. Francis de Sales Parish. Construction of a new church on Water Street began immediately. It was designed as a two-story building for the purpose of providing classroom space on the ground floor and worship space on the second. The new building was dedicated in 1911. The residence at 99 Water Street was purchased as a rectory and 2 Gold Street was bought to serve as a convent for the Ursuline de Jesus Sisters, who were called from France to administer the parish school.

On March 7, 1913, a fire, believed to have been caused by defective wiring, destroyed the new parish building. Reconstruction began almost immediately and the rebuilt church was blessed on November 16, 1913. For unknown reasons the Ursuline de Jesus Sisters were called back to France by their superiors and were replaced by the Ursuline de Merici sisters in 1920. In the early 1920's, the residence at 112 Silver Street was purchased for use as a new Ursuline convent. The parish purchased a parcel of land between Kimball and Preston Streets, and from 1939 to 1967 the Brothers of Christian Instruction administered the St. Joseph School for Boys here.

By the 1960's, the parish of Notre Dame was desirous of a new worshiping facility that would be both larger and more in keeping with the reforms of Vatican II. The St. Joseph School was demolished and ground was broken for a new church on April 5, 1970. One year later the new church building was dedicated.