Polarizing‐Free Triboelectric Dipoles Achieving High Piezoelectric‐Like Sensors

Abstract The fundamental limitation of conventional piezoelectric technologies stems from their intrinsic dipole dependency, where traditional materials (such as ceramics, polymers, and piezoelectric elastomer composites) suffer from mechanical rigidity, inefficient polarizing processes, and compromised electromechanical conversion. Here, a paradigm‐shifting triboelectric dipole architecture is proposed that mimics piezoelectric behaviour through contact electrification. By embedding rationally designed charge‐transfer pairs within elastomer matrices, polarizing‐free triboelectric dipole alignment is achieved with a controlled dipole moment. The self‐powered elastomer exhibited a high piezoelectric‐like coefficient () of 385 pC/N, a low Young's modulus of 0.304 MPa and endogenous electric output (10 V, 90 nA). Subsequent encapsulation ensured voltage retention after water spray and immersion tests. A self‐powered piezoelectric‐like sensor insole based on vertically aligned triboelectric dipole arrays is developed for plantar pressure monitoring. By integrating three‐channel sensing data with a 1D convolutional neural network, it achieved 97.92% accuracy in identifying four gaits (O‐leg, X‐leg, tiptoe walking, normal walking), offering a reliable solution for early‐stage diagnosis. This work establishes a universal design strategy for elastomers that simultaneously achieves low Young's modulus and enhanced electromechanical conversion, opening new frontiers in flexible self‐powered systems for next‐generation wearable healthcare technologies.