A dinuclear metal-organic cage with four acrylate side chains was prepared by self-assembly. Precipitation polymerization of the cage with N-isopropylacrylamide yielded a thermoresponsive nanogel. The host properties of the cage were retained within the gel matrix, endowing the nanogel with the capability to serve as a sorbent for chloride ions in water. Moreover, a heteroleptic cage with the drug abiraterone as co-ligand was integrated into a nanogel. The addition of chloride ions induced a structural rearrangement of the metal-ligand assembly, resulting in the gradual release of abiraterone.