Inherent strength-plasticity tradeoff and unfavorable anti-wear capacity of FCC-structured high-entropy alloys (HEAs) bottlenecks their applications in advanced industries. This work controllably deployed an enhanced heterostructure and graded grain distribution in the single FCC-phase HEA model according to the concept of selective solid solution, which contributed to the ultrahigh compressive strength at appreciable plasticity levels for allowing worn surface to accommodate tribological loading. Simultaneously, the multiscale FCC-coupled architecture with compositional fluctuation effectively inhibits high temperature softening and activates the in-situ tribochemistry protection of the duplex glaze-layer and recrystallized subsurface, reaching low wear between room-temperature and 800 °C. Our alloying strategy offers a novel avenue for further governing mechanical-tribological combined properties in applicable metallic systems. Display omitted