The interfaces introduced in metals by heterostructural design play crucial roles in mechanical behaviors. Here the effect of gradient interfaces on mechanical behavior was investigated in a laminated Cu–30Zn sample composed of coarse-grained and ultrafine-grained layers. Tensile tests revealed a superior strength-ductility synergy with extraordinary strengthening and work hardening. By combining the measurements of height contour and strain distribution using digital image correlation, the development of strain gradient was detected in the near-interface zone during tension, which was caused by the mechanical incompatibilities across interfaces and the synergetic constraint between layers. The intensity of strain gradient in the near-interface zone increased with tensile strain, which was accommodated by the accumulation of geometrically necessary dislocations, thereby resulting in extra back stress and dislocation strengthening.