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The behavior of paint removal with a pulsed laser has been investigated using an NdYAG fiber laser. Experimental and theoretical analyses are conducted to reveal the underlying mechanism of the paint removal. The results show that the depth, radius, and volume of the pit formed by a single pulse become larger with increases in the energy density. The ideal parameters for the complete removal of paint have been achieved. During the paint removal, burning occurred over the surface, and the variation in element content has been attributed t