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Novel carbon microsphere-supported metallic copper nanoparticles (Cu-NP/C) were synthesized using a low-cost and facile method based on carbonising a styrene-based, chelate-forming cation exchange resin loaded with Cu2+ ions. The metal–organic framework served as both copper and carbon source. Cu-NP/C microspheres were characterized by XRD, Raman, SEM, TGA, EDAX, and BET surface area analyser and were employed as heterogeneous catalysts for the reduction of 4-nitrophenol to 4-aminophenol by NaBH4 and for the synthesis of medicinally significant hexahydroquinoline derivatives based on the one-pot, multi-component reaction of aldehydes, dimedone, ethyl acetoacetate, and ammonium acetate. The sustainable and cheap starting material, the relatively easy synthetic procedure, the catalytic efficiency, and the easy separation and reusability of Cu-NP/C microspheres open the door for …