In 1841, Job and Maria Johnson donated land on the southwest corner of College Street and Union Avenue to the Mount Union Methodist Church for the building of this first church. Prior to this time, services were held in the woods during the summer and in a schoolhouse located one and one-half miles east of Mount Union. This structure was built in 1846 and was used by the congregation until it was sold to William A. Nixon in 1857 for $250 and it became a private dwelling. In 1858, the house was moved east on College Street and remained there until the late 1900s as a private residence.

As the congregation increased, the need for a larger building became more apparent. The second church building was built in 1857 on the corner of Hartshorn and Union Avenue at a cost of $1,900. Thomas A. Nixon donated the bell. Mount Union College held its first commencement in it in 1858. By the 1880s the building no longer met the needs of the congregation and was replaced in 1893 by the current brick structure. In the early 1890s, the second church structure was dismantled and became part of the Stroup Lumber Company.

The current church was designed by S. R. Badgely, a prominent architect from Cleveland and constructed in 1893. President William McKinley, then governor of Ohio, assisted at the cornerstone-laying ceremony. The cost of construction was $27,372.54 and the stained glass windows, designed by Flannigan and Biedenweg of Chicago, cost $993.02. The architectural style is Modernized Romanesque and the interior is of the Akron Plan as designed by Lewis Miller.