Elastic materials that store and release elastic energy play pivotal roles in both macro and micro mechanical systems. Uniting high elastic energy density and efficiency is crucial for emerging technologies such as artificial muscles, hopping robots, and unmanned aerial vehicle catapults, yet it remains a significant challenge. Here, a nanocrystalline structure embedded with elliptical martensite nanodomains in ferroelastic alloys was utilized to enable high yield strength, large recoverable strain, and low energy dissipation simultaneously. As a result, the designed Ti–Ni–V alloys demonstrate ultrahigh energy density (>40 MJ m−3) with ultrahigh efficiency (>93%) and exceptional durability. This concept, which combines nano‐sized embryos to minimize energy dissipation of psuedo‐elasticity and employs a fine‐grained structure to enhance yield strength, can be applied to other ferroelastic materials. Furthermore, it holds promise for the development of phase transformation‐involved functionalities such as high‐performance dielectric energy storage, ultralow‐hysteresis magnetostrain, and high‐efficiency solid‐state caloric cooling.