Indium phosphide (InP) quantum dots (QDs) are increasingly considered potent alternatives to traditional cadmium‐based QDs. Notwithstanding, the material stability of InP, especially when juxtaposed with its cadmium‐based counterparts, poses significant challenges in its application. Generally, a thick ZnS shell is applied to InP cores to thwart photo‐oxidation and diminish nonradiative recombination. Yet, the pronounced lattice mismatch between the InP core and the ZnS shell can introduce lattice defects, consequently attenuating the luminescence efficiency. This makes the cultivation of a flawless thick shell a paramount challenge. In the present research, a synthetic methodology is elucidated to fabricate highly efficient InP QDs with dimensions exceeding 20 nm, achieved by alleviating the lattice mismatch strain during the shell growth. By regulating the shell composition and morphology, InP/ZnSe/ZnSeS/ZnS QDs with shield‐like morphology are prepared and demonstrate a photoluminescence quantum yield (PLQY) of ≈90%, exhibiting significantly enhanced photostability and thermal stability. This discovery is expected to greatly advance the preparation of highly efficient InP‐based or other QDs, expanding their potential in various applications such as environmentally friendly displays and energy‐saving lighting.