As the most promising candidate for luminescent semiconductor materials in the future environmentally friendly society, InP nanocrystals (NCs) have attracted strong attention in the past decade. Tremendous efforts have been devoted to address the unstable and poor optical properties of InP NCs for practical applications. An extensive and in‐depth summary of existing literatures can not only provide an important reference for further optimizing of the optical properties of InP NCs, but also lay a foundation for subsequent related applications. In this review, the methods for the synthesis with different P sources and different ZnE (E = Se, S) shells are briefly summarized. The research progress in the optical properties investigation of InP/ZnE and InP/ZnE/ZnE NCs, including absorption, fluorescence, carrier dynamics, and nonlinear optics, are summarized. The relevant applications based on InP/ZnE and InP/ZnE/ZnE NCs are also presented, ranging from light emitting diodes, bioimaging, and solar cells to photocatalytic hydrogen production.