Remote light control of drug release enhances our ability to address the complexity of biological systems because of its remarkable spatial/temporal resolution. Here, a new class of remote-controlled release system by incorporating photoacid generator (PAG) into graphene oxide-capped mesoporous silica was designed for delivering drug payloads to cancer cells via photoinduced pH-jump activation. PAG was immobilized on pore wall of the boronic acid-grafted mesoporous silica via strong physical adsorption, and then the nanoparticle was capped with graphene oxide sheet by an acid-labile boroester bond, leading to the formation of nanogated ensemble (MSP-BA-GO). Illuminating with a UV light, PAG generated a pH jump, which induced cleavage of the boroester linkers and thus resulted in the uncapping of pore gates. Moreover, folic acid-modified, doxorubicin (DOX)-loaded MSP-BA-GO (DOX@MSP-BA-GOF) showed selective cell internalization via receptor-mediated endocytosis and subsequent released DOX by the remote illumination. We envisioned that this remote-controlled drug delivery system could find potential applications for cancer therapy.