4144www.MaterialsViews.com wileyonlinelibrary.com A novel photo-responsive protein-graphene-protein (PGP) capsule that doubles as a photothermal agent with core/shell structure is constructed by anchoring reduced graphene oxide nanosheets on one-component protein (lactoferrin) shell through a double emulsion method. PGP capsules can transport fully concealed hydrophilic anticancer cargo, doxorubicin (Dox), with a large payload (9.43 μmol g −1 ) to be later unloaded in a burst-like manner by photo-actuation triggered by near-infrared irradiation. Being biocompatible yet with a high cancer cell targeting effi ciency, PGP capsules have successfully eradicated subcutaneous tumors in 10 d following a single 5 min NIR irradiation without distal damage. Besides, the photochemothermal therapy of PGP capsules eradicates tumor cells not only in the light-treating area but also widely light-omitted tumor cells, overcoming the tumor recurrence due to effi cient cell killing effi cacy. These results demonstrate that the PGP capsule is a potential new drug delivery platform for local-targeting, ondemand, photoresponsive, combined chemotherapy/hyperthermia for tumor treatment and other biomedical applications.