In the field of construction, the surface of architectural aluminum formwork for concrete pouring will remain the concrete adhesion layer of heterogeneous composite structures. In view of the difficulty of removing the concrete adhesion layer, we studied the technology and mechanism of removing the concrete adhesion layer by laser cleaning technology in this paper. We analyzed the composition and distribution characteristics of residual concrete on the surface of architectural aluminum formwork, set up a laser cleaning test system, carried out laser cleaning experiments on the concrete layer on the surface of architectural aluminum formwork under different storage times, and analyzed the mechanism of removing the concrete adhesion layer by laser cleaning. The experimental results showed that the residual time of concrete will affect the quality and efficiency of laser cleaning concrete residue on the surface of architectural aluminum formwork for concrete pouring. For concrete residues with short residual time, lasering can achieve efficient and high-quality cleaning. A nanosecond pulsed laser could strengthen the surface hardness of the aluminum alloy template during cleaning, which is helpful in improving the durability of the aluminum alloy template. The main mechanisms of laser cleaning to remove the concrete adhesion layer on the surface of architectural aluminum formwork is that the bubbles and water bubbles in the loose structure of concrete instantly absorb high-energy laser and make the concrete aggregate continuously air-burst. This paper provides technological and theoretical support for the application of laser cleaning technology to remove residual concrete on the surface of architectural aluminum formwork for concrete pouring in the field of construction.