The resonance Raman spectrum of InP nanocrystals is characterized by features ascribable to both longitudinal ͑LO͒ and transverse ͑TO͒ optical modes. The intensity ratio of these modes exhibits a strong size dependence. To calculate the size dependence of the LO and TO Raman cross sections, we combine existing models of Raman scattering, the size dependence of electronic and vibrational structure, and electron vibration coupling in solids. For nanocrystals with a radius Ͼ10 Å, both the LO and TO coupling strengths increase with increasing radius. This, together with an experimentally observed increase in the electronic dephasing rate with decreasing size, allows us to account for the observed ratio of LO/TO Raman intensities.