In the present study, a new l-glutamic acid cross-linked chitosan supported on magnetic carboxylic acid-functionalized multi-walled carbon nanotube (FeO/-MWCNT-CS-Glu) nanocomposite was prepared through a convenient one-pot multi-component sequential strategy. Then, nickel nanoparticles (Ni NPs) were entrapped within a matrix of the mentioned nanocomposite. Afterward, the structure of the as-prepared FeO/-MWCNT-CS-Glu/Ni nanosystem was elucidated by various techniques, including FT-IR, PXRD, SEM, TEM, SEM-based EDX and elemental mapping, ICP-OES, TGA/DTA, and VSM. In the next part of this research, the catalytic applications of the mentioned nickel-containing magnetic nanocomposite were assessed upon green one-pot synthesis of diverse heterocyclic frameworks, including bis-coumarins (3a-n), 2-aryl(or heteroaryl)-2,3-dihydroquinazolin-4(1)-ones (5a-r), 9-aryl-3,3,6,6-tetramethyl-3,4,5,6,7,9-hexahydro-1-xanthene-1,8(2)-diones (7a-n), and 2-amino-4-aryl-7,7-dimethyl-5-oxo-5,6,7,8-tetrahydro-4-chromene-3-carbonitriles (9a-n). The good-to-excellent yields of the desired products, satisfactory reaction rates, use of water solvent or solvent-free reaction medium, acceptable turnover numbers (TONs) and turnover frequencies (TOFs), along with comfortable recoverability and satisfying reusability of the as-prepared nanocatalyst for at least eight successive runs, and also easy work-up and purification procedures are some of the advantages of the current synthetic protocols.