AA6061 aluminum/zinc (AA6061/Zn) multilayer composites are fabricated by the accumulative roll bonding (ARB) technique. The microstructure, mechanical properties, and internal friction (IF) of the composites are characterized. The strength increases consistently with the number of rolling cycles, with the highest ultimate tensile strength of ≈300 MPa observed in the ARB6 sample subjected to six cycles and the highest total elongation of ≈11% in the ARB3 sample subjected to three cycles. The amplitude‐dependent IF measured at room temperature indicates that ARB can significantly improve the damping capacity of the composites, and the highest damping value (Q −1 ) of 0.06 was obtained in ARB3 sample at a strain amplitude of 4 × 10 −4 . The high damping of the sample is mainly ascribed to the stress‐induced motion of high‐density geometrically necessary dislocations in pure Zn layers. This study provides an effective and low‐cost strategy of preparing Al strip with high damping capacity and superior mechanical properties.