Methodists in the Smiley area gathered for informal worship services as early as 1879. In 1885 a congregation, originally known as the Bundick Society of the Methodist Episcopal Church South, was organized with about six charter families. The Rev. W. H. Killough served as the church's first itinerate pastor. Later, Rancho circuit and other preachers held services at the Smiley church one a month.
The congregation first met in the Bundick Schoolhouse, a two-story wooden structure also used for Lone Star Masonic Lodge meetings. The Smiley community moved closer to the railroad after the tracks were laid in 1906, and the Methodist congregation built a one-room sanctuary in the new townsite in 1907. It served the fellowship until the current structure was completed and dedicated in 1948.
Members of the Smiley United Methodist Church generally have come from farming and ranching families. Over the years they have provided significant service and leadership to the community and have continued to uphold the ideals and traditions of the founders.