Ionic gels composed of bio-based precursors, such as itaconic acid (IA), are promising for flexible materials. However, IA, a bio-derived monomer for free radical polymerization, faces the challenge of spatial hindrance. Herein, we introduced a choline chloride (ChCl)–IA deep eutectic system to prepare poly deep eutectic solvents (PDESs) as the soft segment and acrylamide (AM) as the precursor of the polymer hard segment to form P(IA-co-AM) ionic gel, driven by hydrogen bonding. Molecular dynamics (MD) well confirms that poly AM (PAM) and ChCl can defeat the spatial resistance caused by −C═C and −COOH of IA. Furthermore, the hard segment PAM provided enhanced strength of the ionic gel trough 21 to 850 kPa. The free volume fraction then demonstrated that the P(IA1-co-AM1.1) ionic gel had both a porous mesh structure and electrical conductivity. This further confirmed that the P(IA-co-AM) ionic gel with high tensile strength, light transmittance, and excellent stability could sense the bending of the human finger and wrist with a gauge factor of 1.82.