A hybrid ultrafiltration membrane based on nanocellulose and zinc oxide nanoparticles (ZnO NPs) was prepared by simple layered filtration without any chemical modification. Microscopic morphology analysis showed that the loading ZnO NPs significantly increased the membrane roughness, and wettability test demonstrated that the membrane surface possessed underwater superoleophobicity. Due to the “puncture effect” of the embedded ZnO NPs, abundant nanochannels were formed in the nanocellulose membrane and the highest water permeance of 5439.7 L·m−2·h−1·bar−1 was achieved. The hybrid membranes exhibited high rejection of nanoparticles larger than 20 nm and macromolecules with molecular weights higher than 100 kDa. Furthermore, ZnO NPs significantly improved the wet tensile strength of membrane. The hybrid membranes achieved high separation efficiency of nano-sized emulsions via size exclusion and demulsification effect, as well as the efficient removal of organic dyes and antibiotics via filtration-adsorption. The combination of underwater superoleophobicity and photocatalytic self-cleaning performance effectively solved the problem of a sharp decrease in permeance caused by oil contamination. This type of nanocellulose/ZnO hybrid membrane, which integrates high permeance, high filtration accuracy, and photocatalytic anti-fouling performance in one design, offers an innovative approach to the preparation of nanocellulose membranes for the treatment of organic wastewater.