Epoxy silane coupling agent A‐187 and amine silane coupling agent A‐1387 were used to modify the interface of carbon‐reinforced aluminum laminates (CARE), respectively. The effects of the type and content of coupling agent on the microstructure and mechanical properties of CARE were investigated. Results show that with the increase in the content of two coupling agents, the wettability first increases and then decreases. When the mass fraction of the two coupling agents is 1%, good wetting property is obtained, and the interlaminar shear and flexural strengths of the CARE plate are the best. Compared with epoxy coupling agent A‐187, amine coupling agent A‐1387 had better wettability to aluminum alloy surface and highly contributed to the improvement of interface structure and properties, which then increased the interlaminar shear and flexural strengths by 19.1% and 8.9%, respectively.