A Fully Natural Gel Matching Synthetic Polymers for Sustainable Flexible Electronics

High‐performance polymers are essential for flexible electronics. However, they rely on non‐renewable petrochemicals and generate non‐degradable waste. Natural alternatives often suffer from poor mechanical properties and processability, generally requiring petroleum‐based modification. Here, a fully natural starch‐based gel (NAG) was fabricated from renewable amylopectin and gelatin, without any petrochemical‐derived components. Through rational design of multiple hydrogen‐bonding networks, the gel exhibits rapid gelation within minutes. It possesses a broad operating temperature window, excellent mechanical properties, robust cryogenic adhesion (∼7.04 MPa on wood), high self‐healing efficiency (∼98%), complete recyclability, electrical conductivity, and biodegradability. The gel precisely detects signals from macroscale strain and temperature to micro‐level physiological changes. It translates micro‐expressions into commands for real‐time remote intelligent vehicle control. This work demonstrates that a fully natural gel can match synthetic gels in performance and multifunctionality. It establishes a universal materials platform for sustainable and intelligent soft electronics with a closed‐loop life cycle.