The research on multiple hydrogen bonds (H‐bonds) hydrogels have gradually aroused wide interest. In this paper, a multiple H‐bonds‐reinforced poly(acrylamide‐co‐2‐vinyl‐4,6‐diamino‐2‐vinyl‐1,3,5‐triazine)/tannic acid (P(Am‐co‐VDT)/TA) hydrogels are prepared. The results suggest that the prepared hydrogel has two types of H‐bonds crosslinking regions: A “soft” region of H‐bonds between the diaminotriazine (DAT) moieties on the polymer chains and the TA pyrogallol/catechol groups, and a “hard” region of H‐bonds forming by DAT moieties with itself. The hard crosslinking region exhibits significantly higher activation energy than the soft region. Such soft and hard dual physically crosslinked networks dramatically enhance the mechanical properties of P(Am‐co‐VDT)/TA hydrogels in a synergistic manner (tensile strength is 2.34 MPa, elongation at break is 410%). Due to the multiple hydrogen bonds, the hydrogel has good pH sensitivity and rapid response to shape memory within a few minutes. In addition, the hydrogels have the capacity of physical adsorption of the anti‐inflammatory drug diclofenac sodium and other molecules with a specific spatially arranged chemical composition. These hydrogels with high mechanical strength, excellent shape memory behavior, and capacity of adsorption of anti‐inflammatory drug could be attractive candidates for applications in the fields of biomedicine, tissue engineering, and medical materials.

The poor adhesion performance of typical gels still remains a challenge to find a simple method to achieve strong and reversible adhesion with the existence of water. Here, a poly(acryloyloxyethyl trimethyl ammonium chloride‐co‐2‐vinyl‐4‐6‐diamino‐1,3,5‐triazine) (P(DAC‐co‐VDT)) gel with high and adjustable interfacial adhesion is fabricated by combining cation‐triazine π interaction and multiple hydrogen bonding and through a one‐pot route. Characterization of the gels reveals that the two types of interactions are introduced into the gel network and that the gel–gel and gel–glass interfacial adhesion can be readily adjusted in a wide range from 15.98 to 123.60 kPa. This approach enables the creation of high‐strength composites using P(DAC‐co‐VDT) gel as matrix, anionic monomer sodium p‐styrene sulfonate as ion concentration adjustor, and discrete quartz sands as filler with easy and repeated moldability and self‐healing capability.