Structural damping composites exhibit considerable potential in aerospace and other fields due to their excellent damping and vibration reduction performance, as well as their structural carrying capacity. However, conventional structural damping composite materials generally do not combine excellent mechanical and damping properties at the same time, which makes it difficult for them to meet the practical demand in engineering. In this paper, polyetherimide (PEI) non-woven fabric interlayer materials loaded with quantified polydopamine (PDA) and carboxylated multi-walled carbon nanotubes (MWCNTs-COOH) were used to prepare carbon fiber-reinforced bismaleimide composites through the co-curing process. The mechanical and damping properties of the composites were systematically studied. The results demonstrate that PEI non-woven fabric interlayers loaded with PDA and MWCNTs-COOH can synchronously improve the mechanical and damping properties of the co-cured composites. The incorporation of carbon nanotubes and polydopamine during the co-curing process synergistically improves the flexural strength, flexural modulus, interlaminar shear strength, and impact fracture toughness of the composites. Most importantly, damping properties show an increase of 45.0% in the loss factor of the co-cured composites. Moreover, the reinforcement mechanism was investigated using the optical microscopy and scanning electron microscopy, which indicated that the PEI interlayers loaded with carbon nanotubes and polydopamine form a rich resin area between the layers of the composites.