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The generation of high-performance heterojunctions between high-strength resin matrix composites and metals is of great significance for lightweight applications in fields such as aerospace and automobile engineering. Herein, we explored the feasibility of employing a laser joining process to achieve high-strength heterojunctions between continuous carbon fiber-reinforced PEEK (CCF30/PEEK) composites and titanium alloy (Ti6Al4V). A joint strength of over 50 MPa was achieved through constructing mechanical interlocking structures between CCF30/PEEK and Ti6Al4V. Tensile tests revealed that the fracture of joints was mainly ascribed to the detachment of carbon fibers from the resin matrix and the breakage of carbon fibers. The structures with different orientations and dimensions were confirmed to significantly influence the formation of interlocking structures near the joining interface and the resultant fracture strength of joints. It is believed that the results presented in this study provide a strong foundation for the production of high-performance heterojunctions.