In this study, a pH-responsive magnetic drug delivery system was prepared by cross-linking of Cofe2O4/graphene oxide to carboxymethyl cellulose (CMC) biopolymer with adipic acid dihydrazide (ADH) and then investigated for loading and release of a poorly water-soluble anti-cancer drug, curcumin (CUR). The CoFe2O4/GO-ADH-CMC bio-nanocomposite was characterized by FE–SEM/EDX, TEM, FT–IR, XRD, TGA, VSM, and zeta-potential techniques. The highest amount of drug loading was achieved as 23.7 mg g–1 at 323 K, pH 6.0, and 120 mg L–1 CUR concentration. The study of adsorption isotherms revealed that the Sips model was best fitted to the equilibrium data (R2 > 0.997), which indicated the contribution of both chemisorption and physisorption in drug loading. Furthermore, the release profile of CUR from drug-loaded CoFe2O4/GO-ADH-CMC was studied in mimicking the endosomal (pH = 5.6) and physiological (pH = 7.4) conditions. After 24 h, the maximum cumulative releases were found to be 86 and 38% at pH = 5.6 and 7.4, respectively. Also, the Peppas-Sahlin kinetic model was followed for the release data. The MTT assay exhibited good biocompatibility of the CoFe2O4/GO-ADH-CMC. The results implied that CoFe2O4/GO-ADH-CMC magnetic bio-nanocomposite might be utilized as a potentially safe carrier with the continuous and slow release of CUR.