In this study, a new type of ceramic composite (PZSC/ZnO) was successfully synthesized using N, P, and S co-doped carbon microspheres derived from polyphosphazene with zinc oxide. The morphology and structure were characterized by Fourier transform infrared spectroscopy, X-ray photoelectron spectroscopy, scanning electron microscopy, energy-dispersive spectroscopy, Raman, X-ray diffraction, BET, and thermogravimetric. Batch experiments were used to explore the adsorption performance under different pH values, initial concentrations, contact times, and temperatures. The results showed that the maximum adsorption capacity of the PZSC/ZnO ceramic composite for uranium was 470.5 mg/g (pH = 5.5, t = 40 min, and T = 25 • C). The adsorption process followed the nonlinear Langmuir model and the pseudo-second-order kinetic model, demonstrating that the monolayered combination of U(VI) with the PZSC/ZnO ceramic composite and the adsorption mechanism was chemical adsorption. Thermodynamic data revealed that the adsorption was a spontaneous endothermic process. Furthermore, P and N may be involved in the adsorption of uranyl ions through binding to the O atoms from ZnO. The main forces between U(VI) and the PZSC/ZnO ceramic composite were attributed to ZnO and heteroatoms doped in the material.