The interface is crucial in determining the properties of laminated metal composites (LMCs). In this study, AA6061/TA1/AA6061 LMCs were produced via hot rolling and subsequent asymmetric cryorolling, followed by aging at 160 °C for 1.5 h. The mechanical properties of the materials were systematically investigated with regard to the impact of the interface during this process. The results demonstrated that the combination of asymmetric cryorolling and aging achieved superior mechanical properties of the composites, yielding a tensile strength of 397 MPa and a uniform elongation of 5.2 %, attributed to the introduced jagged interface and the reduction of interface voids, this procedure notably enhanced the bonding quality of the composites. The bonding strength was improved to 9.06 N/mm, 4.45 N/mm higher than the room temperature rolling + aged sample. Additionally, a more pronounced interface affected zone, approximately 64.7 µm, was noted in the subsequent deformation of the asymmetric cryorolling + aged sample, resulting in higher strain hardening capability. Furthermore, asymmetric cryorolling resulted in higher dislocation density, which maintained a high level even after aging. This phenomenon, along with the precipitated phase formed in the AA6061 layer, contributed to the enhanced strength.