The ultraviolet nanosecond laser surface treatment of carbon fiber-reinforced polymer was studied to optimize surface morphology and enhance bonding strength. The samples were treated with various laser powers and pulse frequencies, and the effects were evaluated using contact angle measurements, surface energy analysis, and mechanical testing. The synergistic mechanisms of photochemical and photothermal effects were revealed, and the influence of energy density on surface morphology was analyzed. The results show that an appropriate energy density (160–203 mJ/cm²) effectively removes epoxy resin, exposes intact carbon fiber surfaces, and significantly improves surface energy and wettability. The water contact angle decreases from 82.7° to 69.7°, and the single lap shear strength increases from 23.6 MPa to 26.7 MPa, with an improvement of 13.1%. However, energy density exceeding 235 mJ/cm² leads to carbon fiber breakage, reducing mechanical performance. This study demonstrates the effectiveness of ultraviolet nanosecond laser treatment in enhancing sample bonding performance, offering an efficient surface treatment solution for applications in aerospace and other demanding fields.