Air self‐charging power systems possess the capability of energy harvesting, conversion and storage simultaneously. However, in general, their self‐charging rate is slow and the batteries cannot be oxidized to the fully charged state due to the weak oxidizability of O2. Herein, we designed an ultrafast air self‐charging aqueous zinc battery by constructing a PANI@Pt/C composite cathode. The introduction of Pt/C catalyst endows the redox reaction between PANI and O2 with fast reaction kinetics and extended redox potential difference. Therefore, the self‐charging rate of the Zn/PANI@Pt/C batteries is effectively accelerated and they can be self‐charged to fully charged state. Furthermore, the PANI can be recharged by O2 simultaneously during discharging process to compensate the consumed electrical energy, achieving prolonged energy supply. In addition, the PANI@Pt/C cathodes can be directly used as the cathodes of flexible self‐charging zinc batteries due to their excellent mechanical properties. As a proof of concept, flexible soft‐packaged Zn/PANI@Pt/C batteries were fabricated and displayed stable electrochemical performance and self‐rechargeability even at different bending states. This work provides a route to design ultrafast chemical self‐charging energy storage devices and broadens the horizons of flexible energy storage devices.This article is protected by copyright. All rights reserved