Anisotropy is the difference in the microstructure or mechanical properties of materials in different directions. Anisotropic behavior occurs in rolled sheets, and this anisotropy is very obvious in laminated composites. In this work, the influence of anisotropy on the microstructure and mechanical properties of Ti/Al laminated composites fabricated by rolling was investigated. The results show that the microstructure and mechanical properties of the Ti/Al laminated composites were obviously anisotropic. The grains in the Al layer of the composites were elongated along the rolling direction and were compressed perpendicular to the rolling direction. The grains in the Ti layer of the composites had no obvious preferential orientation and comprised mainly twins. With the rolling direction as 0°, the mechanical properties of the Ti/Al laminated composites varied greatly as the angle of the composites increased. The tensile strength, elongation and bond strength of the Ti/Al laminated composites decreased with increasing angle of the composites. In addition, the microhardness of the Ti/Al laminated composites increased with increasing angle of the composites.