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Herein, the preparation of a redox\u2010responsive sulfur dioxide (SO<jats:sub>2<\/jats:sub>)\u2010releasing nanosystem, with high SO<jats:sub>2<\/jats:sub>\u2010loading capacity, aimed at improving the treatment efficacy of cancers exhibiting MDR is described. The multifunctional nanomedicine (MON\u2010DN@PCBMA\u2010DOX) is designed and constructed by coating mesoporous organosilica nanoparticles with a zwitterionic polymer, poly(carboxybetaine methacrylate) (PCBMA), which can concurrently load SO<jats:sub>2<\/jats:sub> prodrug molecules (DN, 2,4\u2010dinitrobenzenesulfonylchloride) and chemotherapeutics (DOX, doxorubicin). The generated SO<jats:sub>2<\/jats:sub> molecules can sensitize cells to chemotherapy and overcome the MDR by downregulating the expression of P\u2010glycoprotein. Furthermore, the PCBMA coating prolongs the blood circulation time of the inner core, leading to an increased intratumor accumulation of the nanomedicine. 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