The morphotropic phase boundary (MPB) has been utilized extensively in ferroelectrics and recently been extended to ferromagnets, especially for the magnetostrictive materials. Here, guided by phenomenological theories and phase-field simulations, we proposed a design strategy for obtaining the ultrasensitive magnetoelastic response at the pre-transitional rhombohedral side of ferromagnetic MPB, by further flattening the energy landscape while maintaining large intrinsic magnetostriction. To validate this, we judiciously introduced the light-rare-earth-based $$\hbox {Tb}_{0.1}\hbox {Pr}_{0.9}$$ system to the Co-doped $$\hbox {Tb}_{0.27}\hbox {Dy}_{0.73}\hbox {Fe}_{2}$$ alloy, as $$\hbox {Tb}_{0.1}\hbox {Pr}_{0.9}$$ is an anisotropy compensation system with large intrinsic strains and the transition metal dopant of Co tends to optimize the magnetostriction. Phase-field modeling was used to determine the detailed magnetic domain evolution of the investigated multi-component Laves phase compounds, the results of which were compared with experimental results. At room temperature, an ultrahigh magnetoelastic response $${d}_{33}$$ was found in $$\hbox {Tb}_{0.253}\hbox {Dy}_{0.657}\hbox {Pr}_{0.09}(\hbox {Fe}_{0.9}\hbox {Co}_{0.1})_{2}$$ recompensation system especially at low fields, which is superior to that of the commercial $$\hbox {Tb}_{0.27}\hbox {Dy}_{0.73}\hbox {Fe}_{2}$$ (Terfenol-D) polycrystal. The ultrahigh magnetostrictive sensitivity, together with low raw material cost makes it one of the strongest candidates for magnetostriction applications.
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