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In this study, a copper ferrocyanide/silica/polyvinylidene fluoride (CuFC/SiO2/PVDF) hollow-fiber composite membrane was successfully synthesized through a facile and effective crosslinking strategy. The PVDF hollow-fiber membrane with embedded SiO2 was used to fix the dispersion of CuFC nanoparticles for cesium (Cs) removal. The surface morphology and chemical composition of the composite membrane were analyzed using scanning electron microscopy and X-ray photoelectron spectroscopy (XPS). The composite membrane showed a high Cs rejection rate and membrane flux at the three layers of CuFC and 0.5% SiO2, and its Cs rejection rate was not affected by variation in the pH (pH = 4–10). The modified membrane could be effectively regenerated many times using ammonium nitrate (NH4NO3). The Cs selectivity performance was verified by an efficient Cs rejection rate (76.25% and 88.67% in 8 h) in a solution of 100 μg·L−1 of Cs with 1 mmol·L−1 of competing cations (K+ and Na+). The CuFC/SiO2/PVDF hollow-fiber composite membrane showed a particularly superior removal performance (greater than 90%) in natural surface water and simulated water with a low Cs concentration. Therefore, the CuFC/SiO2/PVDF hollow-fiber composite membrane can be used directly in engineering applications for the remediation of radioactive Cs-contaminated water. Keywords: Cesium removal, Composite membrane, Copper ferrocyanide, Polyvinylidene fluoride