AbstractPortable and wearable electronics are undergoing rapid development, but these flexible devices may break and fail to work under high compressive strains. Here, presented is a new free‐standing compressible carbon nanotube array (CCNA) with a unique gradually crosslinking structure, which mimics the gradient structure of the beak of the giant squid. The CCNAs can tolerate various compressive strains and demonstrate high reversible compressibility up to 1 00 000 cycles with high electrical conductivities. On the basis of the CCNA, a novel all‐solid‐state compression‐sensing supercapacitor (CSS) that can store energy and tolerate and sense the external strain change is produced. It demonstrates a high capacitance of 93.2 mF cm−2 and can be maintained by 94% even after 3000 continuous compressing cycles at a strain of 60%. In addition, it also shows superior strain sensing capability and stability up to 1900 compressive cycles. These flexible CSSs promise a wide range of applications including electronic skins and advanced bioelectronic devices.
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