Technetium and zirconium are two of the most problematic fission products in the PUREX process due to their complex extraction behaviors. Although there are several published works related to the calculation of Tc and Zr distribution coefficients, the reliability of those methods must be validated carefully, and further knowledge in this area is still needed. This work is, therefore, devoted to developing technetium and zirconium distribution coefficient models for predicting their distribution between nitric acid solution and tributyl phosphate in diluent for solutions containing uranium, technetium, and zirconium. The distribution coefficient model for zirconium is based on the organic nitric acid concentration, rather than the free TBP concentration. An improved technetium distribution coefficient model, in the absence of other metals, is also developed. The coextraction of technetium and zirconium or uranium is calculated by ligand exchange mechanisms. The validation results demonstrate that the distribution coefficient models developed in this work are more accurate than established models.