Extra‐Protective‐Layer‐Free Integrated Textile for Robust Protection and Highly Sensitive Bimodal Sensing in Firefighting

Stacking functional layers can integrate protection and sensing into firefighting suits, but excessive layering impedes stimulus transmission, reducing sensitivity. To resolve this, we developed an asymmetric cotton fabric (ACF) via spatially selective deposition: growing a Cu(OH) 2 /Poly(TVPO‐co‐Cyclen) base and asymmetrically depositing polypyrrole. This yields a conductive inner face and a superhydrophobic (WCA = 164.1 ± 5.0°), flame‐retardant (LOI = 30.7%) exterior. This robust protection, elucidated by DFT and IGMH analyses, remains stable even after laundering. By sandwiching a chitosan thermosensitive interlayer (CS) between two ACFs, we fabricated the i‐Textile. Here, the structural asymmetry plays a crucial role: the protective exterior shields the inner sensing layer from water, fire, and conductive contaminants, ensuring long‐term stability. Furthermore, to eliminate electrical crosstalk between capacitive and resistive measurements, we implemented an asymmetric time‐division multiplexing (TDM) strategy. Consequently, the dual‐mode i‐Textile accurately monitors physiological signals (0.25 s; GF = 41.59 N −1 ) and high‐temperature risks (1.89 s; TCR = ‐0.50%·°C −1 ). This work establishes practical structural and circuitry strategies for designing high‐performance firefighting textiles with robust protection and highly sensitive bimodal sensing.