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Father Antonio Ripoll has been credited with the design of the Mission Santa Barbara #4. It is distinguished by its Neoclassical facade consisting of a pediment and engaged columns topped by rudimentary Ionic capitals. General José Figueroa (1792-1835), the Mexican Territorial Governor of Alta California from 1833-1835 supervised the secularization of the Missions on 08/17/1833. Mission land was privatized and sold by the Mexican Government. Despite the secularization, clergy remained at Mission Santa Barbara, operating it as a religious college between 1854-1885. Following the secularization act, Bishop Francisco Garcia Diego y Moreno ordered that all documents generated by all the missions be centrally stored in Santa Barbara. It became the temporary cathedral for the Diocese of Both Californias, created in 1840 and two subsequent administrative regions, the Diocese of Monterey and the Diocese of Monterey/Los Angeles. The mission church's two belltowers indicated that it was a bishop's seat. President Abraham Lincoln returned ownership of the missions to the Catholic Church on 03/18/1865.

The Santa Barbara Mission #4 was made a National Historic Landmark on 10/09/1960. The State of California, Office of Historic Preservation described the mission complex's property: "Santa Barbara Mission was founded December 4, 1786. Portions of five units of its extensive waterworks, built by Indian labor and preserved in this part, are a filter house, Spanish gristmill, sections of aqueducts, and two reservoirs, the larger of which, built in 1806, is used today as part of the city water system. The fountain and lavadero are nearby, in front of the mission, and a dam built in 1807 is located in the Santa Barbara Botanic Garden, one and one-half miles up Mission Canyon. Only ruins remain of the mission's pottery kiln, guard house, and tanning vats." (See "Mission Santa Barbara,"Accessed 10-25-2013.)

The two bell towers were damaged in the Santa Barbara Earthquake (estimated at 6.8 on the Richter Scale) of 06/29/1925 and restored two years later.