We investigated mechanical stress-dependent behaviors of (011)-oriented Mn-doped PIN–PMN–PT single crystals to further improve their stabilities for high-power piezoelectric applications. In contrast to the common belief that mechanical constraint induces depolarization of active piezoelectric materials, the (011)-oriented single crystals demonstrated up to 44% of enhancements in their coercive field when mechanical stress is loaded on the specific flank surfaces of the single crystals. Furthermore, the suggested strategy is also feasible over practical operational temperatures for electroacoustic sensors (5–60 °C), which is beneficial to high-temperature applications. Nevertheless, consistent with the generally accepted trade-off, their electromechanical responses are inevitably degraded at constrained states due to less shear deformation which is key in piezoelectricity of relaxor-PT single crystals. We hope that the current work will elucidate mechanical stress-dependent behaviors of domain-engineered anisotropic relaxor-PT single crystals and provide a clue for a proper selection of prestress levels to achieve better performances of electroacoustic transducers in a variety of environments.