<p>The rapid growth of wearable electronics demands power sources that are not only flexible and durable but also inherently safe. Conventional lithium-ion batteries pose safety risks due to toxic and flammable electrolytes. Aqueous metal-ion batteries offer a promising alternative, yet their application remains limited by poor mechanical compliance, leading to interfacial instability and electrolyte leakage. Here, we report a bionic self-assembly strategy for aqueous zinc-ion batteries using a lipopeptide electrolyte additive named C₁₆K, enabling bulk self-assembly into supramolecular nanohelices to accelerate ion transport and interfacial organization into a dynamic bilayer for interphase regulation. This dual-function synergistically suppresses the formation of Zn dendrites or side reactions, enabling stable Zn plating/stripping. This achieves an ultralong cycling stability and ultrahigh cumulative plating capacity along with a high coulombic efficiency. Therefore, the synergistic reinforcement endows the pouch cell to deliver a high initial capacity, allowing to power electronics in a safe manner. In a following manner, a scorpion tail-inspired bionic flexible battery structure is designed to deliver sustainable energy outputs across various mechanical states using the reinforced systems, effectively powering the wearable multimodal sensors. Our results present a self-assembly strategy using a lipopeptide additive to synergistically reinforce the ions transport and interfacial stability, coordination with a bionic structural design, potentially offering a bioinspired routine for high-performance flexible batteries for wearable electronics.</p>