Laser surface texturing is an effective method to improve the shear strength of the dissimilar joints, and has been widely used in laser joining CFRP to metal. In this work, a femtosecond laser with a wavelength of 515 nm was used to fabricate microstructure on the surface of 2060 Al–Li alloy. And on this basis, high-speed fiber laser joining of CFRP to 2060 Al–Li alloy was realized by a rectangular beam spot, which could provide a relatively uniform energy density. The influence of ablated depth of the microstructure and the scanning line space on the shear strength of dissimilar joints was investigated. The results indicate that the shear strength of the dissimilar joints is greatly improved through femtosecond laser texturing. All the dissimilar joints fail with the mixed failure mode composed of the CFRP matrix fracture and interface fracture. Remarkably, the average shear strength of the dissimilar joints is 35.7 MPa at a relatively high welding velocity of 3.6 m/min and a laser power of 5 kW, which is 2.3 times that of the joint without femtosecond laser texturing.