Diverse industries are witnessing an increase in demand for hybrid structures of metals and carbon-fiber-reinforced thermoplastic composites (CFRTPs). Welding is an essential technique in the manufacture of metal–CFRTP hybrid structures. However, achieving high-strength metal–CFRTP welded joints faces serious challenges due to the considerable disparities in material characteristics. As an effective method to strengthen metal–CFRTP joints, surface texturing on metal is gaining significant attention. This study introduces an emerging surface texturing approach, electrochemical jet machining (EJM) using a film electrolyte jet, for enhancing the performance of AA6061-CF/PA66 hot-pressure-welded (HPW) joints. Parametric effects on surface morphology and roughness in the EJM of AA6061 are investigated. The results show that a rough surface with multiscale pores can be generated on AA6061 by EJM, and that surface morphology can be modulated by adjusting the applied current density and jet translational speed. Subsequently, the effects of different EJM-textured surface morphologies on the performance of HPW joints are examined. Surface textures created by EJM are demonstrated to significantly enhance the mechanical interlocking effect at the bonding interface between AA6061 and CF/PA66, resulting in a substantial increase in joint strength. The maximum joint strength attained in the present work with EJM texturing is raised by 45.29% compared to the joints without surface texturing. Additionally, the joint strength slightly improves as the roughness of EJM-textured surfaces rises, with the exception of rough surfaces that are textured with a combination of low current density and rapid translational speed. Overall, these findings suggest that EJM texturing using a film jet prior to welding is a potential approach for the manufacture of high-performance metal–CFRTP hybrid structures.