ABSTRACT Stimuli‐responsive soft materials capable of converting environmental and physiological stimuli into optical and electrical signals are highly attractive for information security, wearable sensing, and personalized healthcare management. Herein, we report biocompatible viologen‐crosslinked eutectogels derived from poly(hydroxyethyl acrylate) (poly‐HEA) and natural deep eutectic solvent composed of betaine and lactic acid. The eutectogels exhibit high transparency, excellent elasticity,