Ultra‐Tough and Highly Stretchable Dual‐Crosslinked Eutectogel Based on Coordinated and Non‐Coordinated Two Types Deep Eutectic Solvent Mixture

Abstract Eutectogels are gaining attention in flexible device applications for their superior ionic conductivity, stability, biocompatibility, and cost‐effectiveness. However, most existing eutectogels suffer from low strength and toughness. Herein, ultra‐tough and highly stretchable polyacrylamide (PAM) eutectogels featuring a dual‐crosslinked network comprising chemical cross‐linking and physical cross‐linking facilitated by metal coordination bonds and hydrogen bonds are developed. This is achieved through a controlled strategy involving polymerization of acrylamide in a coordinated metal salt‐type deep eutectic solvent (DES) combined with a non‐coordinated choline chloride (ChCl)‐type DES mixture. By varying the molar ratio of these two types of DES, exceptional and adjustable mechanical properties of the resulting eutectogel are achieved, including a high tensile strength ranging from 2.9 to 8.2 MPa and elongation at break ranging from 1725 to 747%, at a 70 wt% DES content. Furthermore, the reversible non‐covalent crosslinking in these eutectogels enables self‐recovery and self‐healing capabilities of eutectogels. The prepared eutectogels also exhibit outstanding ionic conductivity (3.56 mS cm −1 ), making them well‐suited for use as strain sensors in human motion detection. The toughening strategy is universally effective for creating tough eutectogels using coordinated metal salt‐type DES with various metal ions, as well as a diverse range of coordinatable polymers.