In order to develop the single - phase ceramic fuel with good radiation resistance, the UO2-(Zr0.8Ca0.2)O1.8 microspheres with different uranium contents (30mol%, 50mol%, 70mol%) were prepared by Inner-Sol-Gel technique. The technique is with five processes including sol preparation, casting and gelation, washing, drying, and sintering. The parameters of this technique were fixed on the basis of analysis and experiment. The UO2-(Zr0.8Ca0.2)O1.8 spheres were analyzed by XRD. The results show that UO2-(Zr0.8Ca0.2)O1.8 microspheres with different uranium contents (30mol%, 50mol%, 70mol%) were FCC solid solution.