The fabrication, characterization, and therapy efficiency of a noncovalent-bonded hydrogel network, which is assembled by utilizing cucurbit[7]uril as a supramolecular linker to "stick" superparamagnetic γ-Fe2 O3 nanoparticles onto the polymer backbone of catechol-functionalized chitosan are described. The unique barrel-shaped structure of cucurbit[7]uril not only facilitates host-guest recognition with the catechol derivatives, but also forms robust electrostatic interactions between its carbonyl portals and the γ-Fe2 O3 nanoparticles in a supramolecular manner, which leaves the physical and chemical properties of the nanoparticles intact. The γ-Fe2 O3 nanoparticles display vibrational movement and heat generation under an alternating magnetic field, endowing the formed hybrid supramolecular hydrogel with both thermo- and chemotherapy modalities, which are demonstrated both in vitro and in vivo. Here, a facile strategy is introduced to construct noncovalent interactions between a polymer matrix and the incorporated nanoparticles, which is amendable to a wide range of biomedical and industrial applications.