Contrast experiments, in which CFRP and 7075 aluminum alloy stacked materials were drilled with different structure drills respectively, were carried out to assess how process parameters and tools affected hole accuracy, roughness, and burr height as well as cutting force. The results showed that comprehensive cutting ability of the new structure CVD diamondcoated drill was significantly higher than that of the traditional twist drill when drilling CFRP/Al stacks without coolant. The best process parameters were at the speed of 4000 r/min, the feed rate of 0.04 mm/r, with which the aperture accuracy could reach H8, composite shrinkage could be controlled in less than 5 μm and hole wall roughness also meet industry needs (CFRP: Ra≤3.2 μm, Al: Ra≤1.6 μm). Matrix cracking and larger rolled-back burrs would be apparent with the tool wear. On the premise of ensuring the quality and accuracy, the cutting tool could be used for 400 holes at least.