Abstract: In order to improve the problem of the low capacity of uranium in the glass-ceramic form and the difficulty of entering the ceramic phase, the uranium parent glass (PG) and uranium pyrochlore-based glass ceramic (GC) were prepared by a new method combining pretreatment with melt-heat treatment. X-ray diffraction (XRD), scanning electron microscopy (SEM-EDS), transmission electron microscopy (TEM), X-ray photoelectron spectroscopy (XPS) were used to characterize the phase structure of the GC form and evaluate its chemistry stability. The results of XRD show that the uranium pyrochlore in the GC is formed by the phase transformation of the pre-formed fluorite nucleus in the PG and is the main crystalline phase in the GC. The results of SEM and TEM show that the uranium pyrochlore grows uniformly on the glass in a square shape and has good compatibility with glass. The elemental analysis shows that the U in the GC is highly enriched in the pyrochlore phase, and the amount remaining in the glass is extremely small. The EDS results estimate that the stoichiometric formula of uranium pyrochlore is (Ca_1.05Na_0.20U_0.73)(Ti_1.48Al_0.58)O_7+x, in which the capacity of uranium is almost equal to the design value, and the large solid solution of U in ceramic phase is realized. XPS confirms that the valence of U is mostly at +4 both in PG and GC forms, which provides valence feasibility for the capacity of more U in pyrochlore. MCC-1 results show that the GC form has good water resistance.