Abstract

Based on microstructure engineering, graphene oxide (GO)-based piezoresistive pressure sensors have attracted increasing attention due to its amazing sensitivities, but the point-to-point contact mechanism among nanosheets compromises their high-pressure monitoring capabilities. Inspired by the multiple conformations of GO nanosheets, we utilize π-π conjugated interlayer interactions to lock the 3D crumpled conformation of nanosheets, resulting in controllable assembly into a flexible graphene membrane with hierarchically porous structures (PGM). These designed structures include microscale pores formed by the loose stacking of 3D crumpled nanosheets and nanoscale pores supported by densely packed crumples, reaching up to 100 nm in height. The PGM flexible sensor exhibits an unprecedented ultrahigh-pressure response of up to 2000 kPa, with high sensitivities of 1.1 and 0.7 kPa−1 in the pressure ranges of 1–600 kPa and 600–2000 kPa, respectively, and demonstrates over 10,000 cycles of high-pressure stability. Moreover, the PGM flexible sensors enable real-time monitoring of pressure vessel inflation/deflation processes and human activities such as finger, elbow, and knee bending, as well as walking, running, and jumping. This hierarchically porous structure provides a promising avenue for ultra-wide-range and ultra-high-pressure sensing devices, with potential applications in structural health monitoring, personal healthcare, and medical diagnostics.