The two-photon absorption coefficients of crystalline GaAs, InP, CdTe and ZnSe at 1.064 μm and 0.694 μm are calculated by means of a new model which combines the elements of second order perturbation thoery and band structure calculations. A sufficient number of intermediate states are included to assure adequate convergence. This calculational procedure is shown to represent a significant improvement over currently available theoretical models, and the results are in good agreement with available experimental data.