A supramolecular material was prepared by the co-intercalation of FA and DOX into the gallery of Gd3+-doped LDHs. This supramolecular agent was proved to exhibit excellent MRI and FI behavior, as well as chemotherapy toward cancer. The co-intercalated FA enables an efficient and selective drug delivery with good specificity. This work provides a facile approach for the fabrication of a drug formulation with dual-modal imaging and targeted therapy.