A fiber-network chitosan film with three-dimensional interconnected structure was prepared in an alkali/urea solution and regenerated from an ethanol/water coagulation solution. The surface morphology and structure were characterized by scanning electron microscopy (SEM), X-ray diffraction (XRD), N2 adsorption-desorption, attenuated total reflection Fourier transform infrared spectroscopy (ATR-FTIR) and X-ray photoelectron spectroscopy (XPS). Batch adsorption for uranium U(VI) was conducted to investigate the effects of pH, contact time and initial uranium concentration on adsorption capacity. The adsorption of CS-80% was in good agreement with the pseudo-second-order kinetic model and Langmuir isotherm model. The three-dimensional interconnected structure provided more active sites and favored the diffusion of uranium solute, and therefore enhanced the adsorption capacity. The maximum adsorption capacity at pH 5 was 196.735 mg/g. The adsorption mechanism was attributed to chelation and coordination of uranium with -NH2 and -OH groups on chitosan molecules.