The limited capacity of typical materials to resist stress loading, which affects their mechanical performance, is one of the most formidable challenges in materials science. Here, we propose a bone-inspired stress-gaining concept of converting typically destructive stress into a favorable factor to substantially enhance the mechanical properties of elastomers. The concept was realized by a molecular design of dynamic poly(oxime-urethanes) network with mesophase domains. During external loading, the mesophase domains in the condensed state were aligned into more ordered domains, and the dynamic oxime-urethane bonds served as the dynamic molecular locks disassociating and reorganizing to facilitate and fix the mesophase domains. Consequently, the tensile modulus and strength were enhanced by 1744 and 49.3 times after four cycles of mechanical training, respectively. This study creates a molecular concept with stress-gaining properties induced by repeated mechanical stress loading and will inspire a series of innovative materials for diverse applications.