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[Display omitted] • Aerogel-structured MnO 2 was assembled by defect-rich ultrathin nanosheets. • V doping and oxygen vacancies manipulate electronic structure of the MnO 2. • The MnO 2 shows enhanced electrical conductivity and fast Zn2+ diffusion ability. • The MnO 2 cathode presents markedly boosted electrochemical performance. Rechargeable MnO 2 //Zn zinc-ion batteries (ZIBs) gain increasing attention as prospective candidates for large-scale energy storage applications, but MnO 2 cathode materials are afflicted by intrinsic low electrical conductivity, sluggish Zn2+ diffusion kinetics and unstable crystal structure during Zn2+ insertion/extraction. Herein, we report the scalable synthesis of an aerogel-structured MnO 2 (A-MnO 2) assembled by defect-rich ultrathin nanosheets for ZIBs. For the A-MnO 2 , V doping and its induced oxygen vacancies manipulate electronic structure to enhance electrical conductivity and decrease Zn2+ diffusion energy barrier, and meanwhile, the ultrathin nanosheets-assembled aerogel structure favors the exposure of more electrochemically active sites and the shortening of ion diffusion distance. As a consequence, the A-MnO 2 is endowed with markedly boosted electrochemical kinetics and thus superior electrochemical performance than defect-free MnO 2 nanorod counterpart. Furthermore, flexible ZIB devices with both impressive flexibility and outstanding electrochemical properties can be realized using the A-MnO 2 cathode material. This work is expected to promote the practical application of MnO 2 //Zn ZIBs. [ABSTRACT FROM AUTHOR]