In this paper, indium (In)‐rich second‐phase particles are observed in InP crystals, which is induced by the loss of phosphorus (P) during polycrystalline melting. Their characterizations reveal that the size of these In‐rich particles is 200 nm–20 µm. The dislocation structure surrounding the second‐phase particle and its formation is explained by the model of prismatic dislocation loop. The indium‐rich second‐phase particles could be eliminated under P‐rich condition by a rapid in situ P injection before crystal growth. Excessive P injection will lead to the formation of P pores with internal P deposits. The optimal injection value is given to eliminate the defects.