AbstractHydrogels that possess both self‐healing capabilities in tissue engineering and mechanical properties play a pivotal role in advancing flexible sensing and wearable bioelectronic devices technologies. The primary challenge in practical applications revolves around the delicate equilibrium between mechanical properties and self‐regeneration capabilities. Herein, the utilization of conjugated carbonyl compound PI‐COF (Polyimide‐Covalent organic framework) is proposed as reinforcing phases to interact with iron ions, thereby preparing PAA‐based double network hydrogel with high cross‐linking density. Through comprehensive component analysis, it has been determined that the existence of metal coordination bonds, hydrogen bonds along with π–π conjugate system imparts (PAA‐2DC)‐Fe3+/PEDOT: PSS hydrogel excellent self‐healing performance (3rd, 196.2%), elongation (1312%) and tensile strength (71 kPa). Additionally, the hydrogel exhibits remarkable conductivity (σ = 0.5 S m−1), strain sensing sensitivity (GF = 9.3), self‐adhesive properties and demonstrating its ability to differentiate between materials of various sizes and possesses antibacterial properties. These exceptional attributes highlight the potential of the hydrogel in tissue engineering and flexible sensing, simultaneously providing novel research ideas and theoretical basis.