<p>Carbon fiber reinforced polymer (CFRP) composites combined with titanium alloy in laminated structures are prone to defects such as fiber pull-out, tearing, and delamination at the bonding surfaces. These defects arise from the differences in material properties. As a result, they significantly affect the service life and performance of CFRP/TC4 laminated components. Low-frequency vibration drilling technology has been shown to reduce the axial force during drilling and realize effective chip breaking. It is an effective method to improve the quality of lamination structure hole making. This study initially conducts tool adaptability experiments by using chip morphology, hole wall damage, cutting temperature, and hole diameter error as evaluation indicators. Results indicate that the step drill is the optimal tool for machining CFRP/TC4 laminated structures. Subsequently, drilling experiments were conducted using the step drill to analyze the effects of different drilling parameters on drilling performance. Finally, the drilling parameters were optimized using the response surface method and genetic algorithm to obtain the optimal machining parameters.</p>