Metal–organic framework (MOF)-based derivatives are attracting increased interest in various research fields. In this study, nano-cellulose MOF-derived carbon-doped CuO/Fe3O4 nanocomposites were successfully synthesized via direct calcination of magnetic Cu-BTC MOF (HKUST-1)/Fe3O4/cellulose microfibril (CMF) composites in air. The morphology, structure, and porous properties of carbon-doped CuO/Fe3O4 nanocomposites were characterized using SEM, TEM, powder X-ray diffraction (PXRD), X-ray photoelectron spectroscopy (XPS), and vibrating sample magnetometry (VSM). The results show that the as-prepared nanocomposite catalyst is composed of Fe3O4, CuO, and carbon. Compared to the CuO/Fe3O4 catalyst from HKUST-1/Fe3O4 composite and CuO from HKUST-1, this carbon-doped CuO/Fe3O4 nanocomposite catalyst shows better catalytic efficiency in reduction reactions of 4-nitrophenol (4-NP), methylene blue (MB), and methyl orange (MO) in the presence of NaBH4. The enhanced catalytic performance of carbon-doped CuO/Fe3O4 is attributed to effects of carbon preventing the aggregation of CuO/Fe3O4 and providing high surface-to-volume ratio and chemical stability. Moreover, this nanocomposite catalyst is readily recoverable using an external magnet due to its superparamagnetic behavior. The recyclability/reuse of carbon-doped CuO/Fe3O4 was also investigated.