Triboelectric nanogenerator (TENG) has emerged as a novel nanotechnology for energy harvesting and self-powered sensing via utilizing various low-frequency mechanical energies throughout the surrounding environment. However, designing TENG with high physical robustness, flexibility, and output performance is rather challenging. This study develops monolithic conjugated microporous polymer aerogel (CMPA) with delocalized π-conjugation to construct TENG with a robust porous structure. The as-produced CMPA is composed of hollow intertwined nanotubes with a high degree of flexibility and high specific surface area (up to 528 m2 g−1). Due to its intrinsic nature of conjugated electron transfer and architectural characteristics, the CMPA-based TENG (effective area: 4.9 cm2) shows a high sensitivity to mechanical force and excellent electric output (open-circuit voltage: 72 V, short-circuit peak current: 3.2 µA and transferred charge: 48 nC). Moreover, the CMPA-based TENG can charge micro-electronic devices and sense human motions. This work will inspire the design of aerogel-based electronic devices and the management of renewable energy resources.