The vandalism was the latest in a string of attacks against statues of the Franciscan priest at missions throughout California, including in San Fernando and Santa Barbara.
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Serra was a Catholic priest of the Franciscan order in the late 1700s who is seen as a key figure in the Spanish colonization of California. He founded nine of California's 21 missions and was made a saint in 2015.
Some Native American groups criticized his selection for sainthood for his association with the killing and mistreatment of their ancestors in that era.
Red paint was splashed across the front of the Serra statue around 1:15 a.m. Friday. Surveillance video shows the suspect also trying to cut off the statue's head with a saw, but failing and just leaving a gash on the side.
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"Whenever any damage is done to the mission, it hurts us. It pains us," said the mission's Father Tony Diaz.
Added Sister Brigid: "It's a horrible thing. Whoever it is has a great deal of hate in him or animosity."
Police were seen gathering evidence at the scene and characterized the vandalism as a hate crime. The cost of the damage was estimated at $2,000.