A series of new complexes of Schiff base 2-bromo-1N-[4-N,N-bis(2′; -cynoethylaminobenzalidene)]aminobenzene (BCABAB) have been prepared from thorium(IV) and dioxouranium(V) metal salts having composition UO 2X2.nL (X = CH3COO-, NO 3-, I- or NCS-, n = 2; X = ClO 4-, n = 4; L = BCABAB) and ThX4.nL (X = NO 3-, NCS-, n = 2, X = I-; n = 4 and X = ClO4-; n = 6, L = BCABAB). BCABAB acts as neutral monodentate ligand and coordinate to the metal ion via azomethine nitrogen.