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Police said Jesus Acevedo, 27, was spotted on surveillance video Tuesday night putting gas on the building.
He then lit a match and the wall went up in flames, police said.
ABC11 was the only news crew there when Acevedo was arrested Wednesday.
Church members were inside the building at the time of the fire, but were able to get out without any injuries.
Investigators said they believe Acevedo attended service at the church Sunday, and then tried to break into the daycare Monday while children were inside.
He is charged with first-degree arson and is being held at the Cumberland County Detention Center on a $25,000 secured bond.