CoFe2O4@SiO2@APTES@HO-PBA@Cu(OAc)2: A magnetic core-shell copper-based nanocatalyst was suc-cessfully prepared. The fabricated nanocatalyst was structurally authenticated using various analytical techniques such as FT-IR, XRD, SEM, TEM, EDS, ICP-AES, TGA/DTA, XPS, BET, and VSM. The highly pro-ficient catalyst proved its dependability for one-pot synthesis of diester/methyl-substituted polycyclic fused 1,5-benzodiazepines via three-component domino reaction of nucleophilic addition and elimina-tion, Michael addition, C-C cross-coupling reactions, and H proton transfer reaction in good to excellent yields. Also, all products were obtained in high TON (up to 17,241) and TOF (up to 4816), which reveals the nanocatalyst has high activity and selectivity in described domino reactions. The suggested mech-anism for one-pot synthesis of diester/methyl-substituted polycyclic fused 1,5-benzodiazepines in the presence of copper-based nanocatalyst was also proposed, respectively. The nanocatalyst can be reused seven times without significant loss of its catalytic efficiency. The easy recovery of the nanocatalyst and reusability, broad substrate scopes, short reaction time, high yields of products, and mild conditions make this protocol practical, environmentally friendly, and economically attractive.(c) 2022 Elsevier Ltd. All rights reserved.