The synergy of tribology design and surface engineering is vitally important for fulfilling the long-term anti-wear requirements of mechanical equipment. Here, Q345 steel was processed by shot peening (SP) for forming a volcano-like hardened layer (77.72 HV) with high surface roughness (3.77 μm) and low residual tensile stress (210.75 MPa). Then, a zinc-rich epoxy coating was painted on SP-strengthened Q345 steel to construct the double-layer protection. The double-layer system shows excellent tribological behaviors, especially wear resistance being reduced by 76.50% and 38.75%, respectively, with Q345 steel and that sprayed by epoxy coating as a comparison. Crucially, SP layer plays a role in mechanical support, while epoxy coating acts as a cushion to friction force, thus achieving the synergy for enhancing the anti-friction/wear abilities.