Nonstoichiometric solid solutions in the system UO2‐ThO2 were formed by sintering U3O‐ThO3 and codigested nitrate mixtures in air. The oxygen content of the solid solutions was determined by a weight‐loss method. The changes occurring in oxygen content during solid solution formation and densification were determined for a 70.4 mole % UO2‐29.6 mole % Tho2 composition formed by sintering U3O3‐ThO2 in air. The first evidence of solid solution occurred at 1000° C. and solution was complete above 1250°C. Thermal cycling of solid solutions in air showed a minimum oxygen‐uranium ratio of 2.34 for the compositions studied. The minimum oxygen‐uranium ratio obtained during thermal cycling decreased with increasing Tho2 content.