The emergence of stretchable textile‐based mechanical energy harvester and self‐powered active sensor brings a new life for wearable functional electronics. However, single energy conversion mode and weak sensing capabilities have largely hindered their development. Here, in virtue of silver‐coated nylon yarn and silicone rubber elastomer, a highly stretchable yarn‐based triboelectric nanogenerator (TENG) with coaxial core–sheath and built‐in spring‐like spiral winding structures is designed for biomechanical energy harvesting and real‐time human‐interactive sensing. Based on the two advanced structural designs, the yarn‐based TENG can effectively harvest or respond rapidly to omnifarious external mechanical stimuli, such as compressing, stretching, bending, and twisting. With these excellent performances, the yarn‐based TENG can be used in a self‐counting skipping rope, a self‐powered gesture‐recognizing glove, and a real‐time golf scoring system. Furthermore, the yarn‐based TENG can also be woven into a large‐area energy‐harvesting fabric, which is capable of lighting up light emitting diodes (LEDs), charging a commercial capacitor, powering a smart watch, and integrating the four operational modes of TENGs together. This work provides a new direction for textile‐based multimode mechanical energy harvesters and highly sensitive self‐powered motion sensors with potential applications in sustainable power supplies, self‐powered wearable electronics, personalized motion/health monitoring, and real‐time human‐machine interactions.

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Developing advanced heterogeneous catalysts with atomically dispersed active sites is an efficient strategy to boost the kinetics of peroxymonosulfate (PMS) activation for micropollutant removal. Here, we report a binary Mo2TiC2T x MXene-based electroactive filter system with abundant surface Mo vacancies for effective activation of PMS. The Mo vacancies assumed two essential roles: (i) as anchoring sites for Fe single atoms (Fe-SA) and (ii) as cocatalytic sites for the Fenton-like reaction. Fe-SA formed strong metal–oxygen bonds with the Mo2TiC2T x support, stabilizing at the sites previously occupied by Mo. The resulting Fe-SA/Mo2TiC2T x nanohybrid filter achieved 100% degradation of sulfamethoxazole (SMX) in the single-pass mode (hydraulic retention time <2 s) when assisted by an electric field (2.0 V). The rate constant (k = 2.89 min–1) for SMX removal was 24 and 67 times greater than that of Fe nanoparticles immobilized on Mo2TiC2T x and the pristine Mo2TiC2T x filter, respectively. Operation in the flow-through configuration outperformed the conventional batch reactor model (k = 0.17 min–1) due to convection-enhanced mass transport. The results obtained from experimental investigations and theoretical calculations suggested that atomically dispersed Fe-SA, anchored on Mo vacancies, was responsible for the adsorption and activation of PMS to produce sulfate radicals (SO4 •–) in the presence of an electric field. This study provides a proof-of-concept demonstration of an electroactive Fe-SA/Mo2TiC2T x filter for broader application in the treatment of water contaminated by emerging micropollutants.