ABSTRACT: The Ce-Mn binuclear LDH was prepared at four different molar ratios of Ce to Mn (1:1, 1:2, 1:3, and 1:4), modified with both 3-chloropropyltrimethoxysilane (CPTMS) and N-amino-phthalimide (NAP), complexed with Cu(II), and characterized by the FT-IR, ICP, XPS, XRD, BET, UV/Vis, EDX, SEM, SEM-mapping, TEM, and TGA-DTA techniques. The ICP, XPS, BET, and UV-vis techniques showed that the 1:4 molar ratio of Ce to Mn is the best, therefore it was used as a heterogeneous nanocatalyst for the green synthesis of fourteen spiro[acridine-indole]triones from the three-component condensation reaction of isatin, aniline, and 1,3-diketone in mild reaction conditions. The advantages of this method include the absence of harmful organic solvents, easy separation of the catalyst and products, and rapid achi