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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 Tb 0.1 Pr 0.9 system to the Co-doped Tb 0.27 Dy 0.73 Fe 2 alloy, as Tb 0.1 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 Tb 0.253 Dy 0.657 Pr 0.09 (Fe 0.9 Co 0.1) 2 recompensation system especially at low fields, which is superior to that of the commercial Tb 0.27 Dy 0.73 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. [ABSTRACT FROM AUTHOR]