Ultra‐Sensitive, Decoupled Multimodal Sensing via Dual‐Network Iontronic Organohydrogels

Flexible sensors capable of mimicking human skin's multimodal perception are highly desired for wearable electronics. However, achieving inherently decoupled detection of multiple physical stimuli in a single device remains a fundamental challenge. Here, a polyacrylamide/polyvinyl alcohol/glycerol/calcium chloride (PAM/PVA/Gly/CaCl 2 , PPGC) dual‐network ionic organohydrogel is integrated into a stacked architecture that physically separates capacitive pressure sensing from resistive temperature and strain sensing, enabling inherent signal decoupling. The dual‐network structure, together with Gly‐induced hydrogen bonding, endows the organohydrogel with robust mechanical properties, anti‐drying capability, and self‐healing behavior. The capacitive pressure sensor achieves an ultrahigh sensitivity of 9426 kPa −1 in the low‐pressure regime and response/recovery times as fast as 20 ms. The resistive temperature sensor exhibits a linear response from 20°C to 100°C with a temperature coefficient of resistance of −0.269°C −1 . Cross‐decoupling experiments confirm negligible interference between pressure and temperature signals. Practical demonstrations include gesture recognition using a five‐channel array, real‐time breath monitoring for apnea screening, and spatial mapping of simultaneous pressure and temperature stimuli with a 4 × 4 sensor array. This strategy provides a promising platform for advanced wearable health monitoring and human‐machine interaction.