RuO₂ is one of the benchmark electrocatalysts used as the anode material in proton exchange membrane water electrolyser. However, its long‐term stability is compromised due to the participation of lattice oxygen and metal dissolution during oxygen evolution reaction (OER). In this work, weakened covalency of Ru−O bond was tailored by introducing tensile strain to RuO₆ octahedrons in a binary Ru−Sn oxide matrix, prohibiting the participation of lattice oxygen and the dissolution of Ru, thereby significantly improving the long‐term stability. Moreover, the tensile strain also optimized the adsorption energy of intermediates and boosted the OER activity. Remarkably, the RuSnO_x electrocatalyst exhibited excellent OER activity in 0.1 M HClO₄ and required merely 184 mV overpotential at a current density of 10 mA cm⁻². Moreover, it delivered a current density of 10 mA cm⁻² for at least 150 h with negligible potential increase. This work exemplifies an effective strategy for engineering Ru‐based catalysts with extraordinary performance toward water splitting.

The design and fabrication of flexible, porous, conductive electrodes with customizable functions become the prime challenge in the development of new‐generation wearable electronics, especially for rechargeable batteries. Here, the NiCo bialloy particulate catalyst‐loaded self‐supporting carbon foam framework (NiCo@SCF) as a flexible electrode has been fabricated through one facile adsorption‐pyrolysis method using a commercial melamine foam. Compared with the electrode with Pt/C and Ir/C benchmark catalysts, the NiCo@SCF electrode exhibited superior bifunctional electrocatalytic performance in alkaline media with a half‐wave potential of 0.906 V for oxygen reduction reaction, an overpotential of 286 mV at j = 10 mA cm⁻² for oxygen evolution reaction, and stable bifunctional performance with a small degradation after 20,000 voltammetric cycles. The as‐assembled aqueous zinc–air battery (ZAB) with NiCo@SCF as a self‐supporting air cathode demonstrated a high peak power density of 178.6 mW cm⁻² at a current density of 10 mA cm⁻² and a stable voltage gap of 0.94 V over a 540 h charge−discharge operation. Remarkably, the as‐assembled flexible solid‐state ZAB with self‐supporting NiCo@SCF as the air cathode presented an engaging peak power density of 80.1 mW cm⁻² and excellent durability of 95 h undisrupted operation, showing promise for the design of wearable ZAB. The demonstrated electrode fabrication approach exemplifies a facile, large‐scale avenue toward functional electrodes, potentially extendable to other wearable electronics for broader applications.