This article presented a facile two-step hydrothermal strategy to anchor the Fe 3 O 4 nanoparticles on the surface of Zn Al LDH nanosheets, and investigated systematically the potential application of the constructed Fe 3 O 4 /Zn-Al LDH nanocomposites in the biomedical field of controlled drug delivery. It was revealed that the formed Fe 3 O 4 /Zn-Al LDH nanocomposites exhibited uniform mesopores, high surface area of 121.7 m2/g, good superparamagnetism and appropriate saturation magnetization of 40.7 emu/g. Due to these fascinating properties, this work explored the application of Fe 3 O 4 /Zn-Al LDH in the field of nanocarrier using the doxorubicin hydrochloride (DOX) as a model anticancer drug for the detailed investigations of drug loading capacity, controlled release behavior and cytotoxic effects under in vitro conditions. The Fe 3 O 4 /Zn-Al LDH showed a good drug storage capacity and a pH-responsive drug release profile. After loading the anti-cancer drugs, the DOX-loaded Fe 3 O 4 /Zn-Al LDH exhibited enhanced therapeutic effect on human hepatocellular carcinoma cells (HepG2), demonstrating that the fabricated Fe 3 O 4 /Zn-Al LDH nanocomposites have a great potential in cancer therapy. • Anchoring the Fe 3 O 4 nanoparticles on the surface of Zn Al LDH nanosheets. • Uniform mesopores, high specific surface area and superparamagnetic behavior. • Promising potential of constructed Fe 3 O 4 /Zn-Al LDH as a drug delivery vehicle. • A good drug storage capacity and a pH-responsive drug release profile. [ABSTRACT FROM AUTHOR]