The new developed metal/composite co-cured material composed of carbon fiber–reinforced plastic and Al phases has been increasingly applied for manufacturing of attitude control flywheel in aerospace industry. However, drilling of co-cured material is still a challenging task to produce holes with high quality and low cost in the assembly chain and dynamic balance debugging of attitude control flywheel. In other words, the relevant mechanisms and experimental findings involved in the drilling process of carbon fiber–reinforced plastic/Al co-cured material is not clearly defined, which impedes the progress of attitude control flywheel production. To this end, this article specially addresses the experimental studies on the drilling process of carbon fiber–reinforced plastic/Al co-cured material with standard TiAlN-coated cemented carbide twist drill. The significance of this work aims to reveal the regardful cutting responses of the hole characteristics and tool wear modes during the practical drilling process of co-cured material. A full factorial experiment including three levels of feed rate and four levels of cutting speed was performed. The hole diameter shows different values in different positions while it indicates consistent pattern regardless of the cutting variables: the largest in the Al phase, followed by the upper and lower carbon fiber–reinforced plastic phases, respectively. Grooves and matrix degradation are the major machining defects for carbon fiber–reinforced plastic layers, while a great chip debris adhered to the machined surface is the case for Al layer. Subsequent wear analysis showed that abrasion was mainly maintained at the vicinity of major/minor cutting edges and drill edge corner, followed by chip adhesion on the chisel edge region. Carbide substrate of drill flank face is exposed, and thereafter cavities are formed under the strong mechanical abrasion. These results could provide several implications for industrial manufacturers during the attitude control flywheel production.