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Stimulus‐responsive drug release possesses considerable significance in cancer therapy. This work reports an upconversion‐luminescence‐fueled DNA–azobenzene nanopump for rapid and efficient drug release. The nanopump is constructed by assembling the azobenzene‐functionalized DNA strands on upconversion nanoparticles (UCNPs). Doxorubicin (DOX) is loaded in the nanopump by intercalation in the DNA helix. Under NIR light, the UCNPs emit both UV and visible photons to fuel the continuous photoisomerization of azo, which acts as an impeller pump to trigger cyclic DNA hybridization and dehybridization for controllable DOX release. In a relatively short period, this system demonstrates 86.7 % DOX release. By assembling HIV‐1 TAT peptide and hyaluronic acid on the system, targeting of the cancer‐cell nucleus is achieved for perinuclear aggregation of DOX and enhanced anticancer therapy. This highly effective drug delivery nanopump could contribute to chemotherapy development.

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Stimulus-responsive drug release possesses considerable significance in cancer therapy. This work reports an upconversion-luminescence-fueled DNA-azobenzene nanopump for rapid and efficient drug release.T he nanopump is constructed by assembling the azobenzene-functionalized DNAs trands on upconversion nanoparticles (UCNPs). Doxorubicin (DOX) is loaded in the nanopump by intercalation in the DNAhelix. Under NIR light, the UCNPs emit both UV and visible photons to fuel the continuous photoisomerization of azo,w hich acts as an impeller pump to trigger cyclic DNA hybridization and dehybridization for controllable DOX release.I narelatively short period, this system demonstrates 86.7 %D OX release.B ya ssembling HIV-1 TATp eptide and hyaluronic acid on the system, targeting of the cancer-cell nucleus is achieved for perinuclear aggregation of DOXa nd enhanced anticancer therapy. This highly effective drug delivery nanopump could contribute to chemotherapyd evelopment.Chemotherapy remains the principal clinical antitumor strategy. [1] However,i to ften results in grievous toxic side effects due to the uncontrollable dose. [2] Stimulus-responsive drug-release systems can enhance drug accumulation in tumor tissues and eliminate off-target toxicity. [2b, 3] Azobenzene (azo), which can reversibly isomerizes between cis and trans form under visible (Vis) and UV irradiation, [4] has been assembled on the surface of mesoporous nanoparticles [5] and microporous multilayer films [6] to act as ap hotoresponsive trigger for controlled drug release.To improve release efficiency, some pump-type switchers [7,8] have been designed to accelerate the drug-release process.W ith the capability of simultaneously emitting photons in both UV and Visr egions upon near-infrared (NIR) irradiation, [9] upconversion nanoparticles (UCNPs) have been modified with azo [10] to continuously transform azo back and forth to propel drug release. [10a] In these UCNPs-azo nanodevices, [4a, 10] azo is usually isolated from UCNPs,w hich weakens the luminescence-fueled efficiency.Therefore,these strategies need al ong exposure time to release ad rug in asatisfactory amount, which results in at hermal injury from continuous point-fixed irradiation.To overcome this drawback, this work used azo-functionalized DNAs trands to design an anopump for efficient and controllable drug release.F lexible DNAc hains could be compactly assembled on UCNPs [11] to act as the pump-type switcher triggered by the reversible conformational change of azo,w hich is conveniently fueled by Visa nd UV irradiation emitted from the UCNPs.M oreover,t he anticancer drug doxorubicin (DOX) could be selectively intercalated in as pecific DNAh elix [12] for highly efficient loading (Scheme 1a). Thec ontinuous rotation-inversion movement of the phenyl moiety of azo in the hybridization zone of DNA backbones (DNAs trands LA Azo ,L C Azo with 3azo moieties per DNAstrand) determined the feasibility of the molecular impeller pump via DNAhybridization [13] and dehybridization to controllabl...