Raman spectra of gallium phosphide (GaP) nanosolids (unheated and heat-treated at 598 and 723 K, respectively)were investigated. It was observed that both the longitudinal optical mode (LO) and the transverse optical mode (TO) displayed an asymmetry on the low-wavenumber side. The scattering bands were fitted to a sum of four Lorentzians which were assigned to the LO mode, surface phonon mode, TO mode, and a combination of Ga-O-P symmetric bending and sum band formed from the X-point TA + LA phonons, respectively. Analysis of the characteristic of surface phonon mode revealed that the surface phonon peak of the GaP nanosolids could be confirmed. In the infrared spectrum of the GaP nanoparticles, we observed the bands on account of symmetric stretching and bending of PO2, as well as stretching of Ga-O.The Raman scattering intensity arising from the Ga-O-P linkages increased as increasing the heat-treatment temperature.