With the booming development of flexible electronics, the need for a multifunctional and high-performance strain sensor has become increasingly important. Although significant progress has been made in designing new microstructures with sensing capabilities, the tradeoff between sensitivity and workable strain range has prevented the development of a strain sensor that is both highly sensitive and also stretchable. Here, a wrinkle-assisted crack microstructure is designed and fabricated via prestretching the multiwalled carbon nanotubes ink (CNTs ink)/polyurethane yarn (PU yarn). This designed structure originates from the mismatch in Young’s modulus and elasticity between the CNTs ink and PU yarn during the stretching process. The structure endows the sensor with combined characteristics of a high sensitivity toward stretching strain (gauge factor of 1344.1 at 200% strain), an ultralow limit of detection (<0.1% strain), excellent durability (>10 000 cycles), a wide workable strain range (0–200%), and outstanding response and stability toward bending deformation. This high-performance strain sensor will see widespread improved performance across applications such as intelligent fabrics, electrical skins, and fatigue detection for full-range human motion monitoring.

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Smart skin is highly desired to be ultrasensitive and self‐powered as the medium of artificial intelligence. Here, an ultrasensitive self‐powered mechanoluminescence smart skin (SPMSS) inspired by the luminescence mechanism of cephalopod skin and the ultrasensitive response of spider‐slit‐organ is developed. Benefitting from the unique strain‐dependent microcrack structure design based on Ti3C2Tx (MXene)/carbon nanotube synergistic interaction, SPMSS possesses excellent strain sensing performances including ultralow detection limit (0.001% strain), ultrahigh sensitivity (gauge factor, GF = 3.92 × 107), ultrafast response time (5 ms), and superior durability and stability (>45 000 cycles). Synchronously, SPMSS exhibits tunable and highly sensitive mechanoluminescence (ML) features under stretching. A relationship between ML features, strain sensing performances, and the deformation has been established successfully. Importantly, the SPMSS demonstrates excellent properties as triboelectric nanogenerator (4 × 4 cm2), including ultrahigh triboelectric output (open‐circuit voltage VOC = 540 V, short‐circuit current ISC = 42 µA, short‐circuit charge QSC = 317 nC) and power density (7.42 W m−2), endowing the smart skin with reliable power source supply and self‐powered sensing ability. This bioinspired smart skin exhibits multifunctional applications in health monitoring, visual sensing, and self‐powered sensing, showing great potential in artificial intelligence.

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