As an emerging energy technology, hygroelectric generators can use the energy of environmental moisture to generate electricity. They have attracted considerable attention from researchers in the field of green energy. We prepared a biofilm-based hygroelectric generator on an ITO-conductive glass substrate based on the whole-cell Geobacter sulfurreducens (Gs) in the early stage (b-HEG), which exhibits excellent power-generation performance. However, the monotonous, rigid structure severely limits its application under complex working conditions. In this study, a b-HEG with a fast self-healing function and high flexibility was successfully prepared based on the Gs film and flexible substrate PET–ITO. The generator (1 cm²) can generate 0.65 V of open-circuit voltage, 6.4 μA of short circuit current, 1.087 μW/cm² of output power density, and continuously generate power for >48 h without attenuation. The b-HEG has the characteristics of arbitrary folding and bending and rapid self-healing. It can recover 100% of its flexibility and power-generation capacity within 1.5 min after the loss of power-generation function by cutting off the biofilm. Additionally, it can be self-healed in multiple cycles to avoid the failure of the device due to deformation or fracture damage in the future working process. Further, it can realize the sustainable power-generation function of the device in a complex working environment. At the same time, the generator has a simple manufacturing process, low cost, zero pollution, and zero carbon emissions, which is of great significance for the development of global carbon neutrality and green energy technologies.

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