The transferability of structure–property relationships for laser-pretreated metal adhesive joints to laser-pretreated metal–carbon-fiber-reinforced plastic (CFRP) bonds was investigated. Single-lap shear tests were performed on hybrid AW 6082-T6–CFRP specimens pretreated with the same pulsed laser surface parameter sets on the metal surface as previously tested, AW 6082-T6–E320 metal adhesive joints. The fracture surfaces were characterized to determine the type of failure and elucidate differences and commonalities in the link between surface structures and single-lap shear strengths. Digital image analyses of the hybrid specimens’ fractured surfaces were used to quantify remaining CFRP fragments on the metallic joint side. The results indicate that high surface enlargements and the presence of undercut structures lead to single-lap shear strengths exceeding 40 MPa and 35 MPa for unaged and aged hybrid specimens, respectively. Whereas for the metal–polymer joints, the trend from high strength to weakly bonded specimens is largely continuous with the degree of surface structuring, hybrid metal–CFRP joints exhibit a drastic drop in joint performance after aging if the laser-generated surface structures are less pronounced with low surface enlargements and crater depths. Surface features and hydrothermal aging determine whether the specimens fail cohesively or adhesively.