LAUSR

While state‐of‐the‐art skin‐adhering fibrous electrodes have distinct benefits in personal wearable bioelectronics, considerable challenges persist in the production of fibrous‐based soft conductive biosensing nanomaterials and their integration into efficient multisensing platforms. Here, an electrochemical‐electrophysiological multimodal biosensing patch based on MXene/fluoropolymer nanofiber‐derived hierarchical porous TiO2 nanocatalyst interconnected 3D fibrous carbon nanohybrid electrodes is reported. The nanohybrid electrode is produced via a one‐step laser carbonaceous thermal oxidation, resulting in excellent elctroconductivity (sheet resistance = 15.6 Ω sq−1), rich active edges for effective electron transmission, and abundant support for enzyme immobilization. The features are attributed to three synergistic effects: i) conductivity of the interior, unoxidized MXene layers, ii) quick heterogeneous electron transmission of the exterior TiO2 nanoparticles, and iii) the porous disordered carbon's electron “bridge” effects. Based on the foregoing, the nanohybrid modified biosensing patch integrated into textile is demonstrated to be capable of simultaneously and precisely monitoring sweat glucose with pH adjustment (sensitivity of 77.12 µA mm−1 cm−2 within physiological concentrations of 0.01–2 × 10−3 m) and electrocardiogram signals (signal‐to‐noise ratio = 37.63 dB). This novel approach paves the way for controlled investigations of the nanohybrid, for several functionalization and design options, and for the mass manufacturing capabilities required in real‐world applications.