Phase relations in the systems NpO2–ZrO2 and CaO‐stabilized zirconia–NpO2 were studied for the suitability of immobilization of minor actinide neptunium in crystalline zirconia‐based waste forms. Phase studies of NpO2–ZrO2 system were studied for the first time. The solid‐state reaction between NpO2 and ZrO2 in air at 1400°C showed the formation of ZryNp1‐yO2 type of phases having single‐phase fluorite, single‐phase tetragonal, and a mixture of fluorite and tetragonal solid solutions for zirconium concentration ranges 0
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