InP nanocrystals synthesized by refluxing and annealing of organic solvent are determined from XRD measurements to have an average granularity of 25 nm. The nonlinear optical properties of the InP nanocrystals studied by using laser Z-scan technique with 50ps pulses at 532nm are found to reveal strong nonlinear optical properties and two-photon absorption phenomenon. Also, the nonlinear absorption coefficient, the nonlinear refractive index and the third-order nonlinear optical susceptibility are determined by experiments, in which the nonlinear refractive index is three orders of magnitude larger than that of bulk InP.