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A facile approach was successfully developed for synthesis of cellulose nanocrystals (CNC)-supported magnetic CuFe₂O₄@Ag@ZIF-8 nanospheres which consist of a paramagnetic CuFe₂O₄@Ag core and porous ZIF-8 shell. The CuFe₂O₄ nanoparticles (NPs) were first prepared in the presence of CNC and dispersant. Ag NPs were then deposited on the CuFe₂O₄/CNC composites via an in situ reduction directed by dopamine polymerization (PDA). The CuFe₂O₄/CNC@Ag@ZIF-8 nanocomposite was characterized by TEM, FTIR, XRD, N₂ adsorption-desorption isotherms, VSM, and XPS. Catalytic studies showed that the CuFe₂O₄/CNC@Ag@ZIF-8 catalyst had much higher catalytic activity than CuFe₂O₄@Ag catalyst with the rate constant of 0.64 min^−1. Because of the integration of ZIF-8 with CuFe₂O₄/CNC@Ag that combines the advantaged of each component, the nanocomposites were demonstrated to have an enhanced catalytic activity in heterogeneous catalysis. Therefore, these results demonstrate a new method for the fabrication of CNC-supported magnetic core-shell catalysts, which display great potential for application in biocatalysis and environmental chemistry.