<p>The fabrication of polyacrylamide (PAM)-based functional hydrogels containing renewable material represents a promising exploration for treating organic dye and adhesive applications. This research fabricated the hydrogels composed of poly-(acrylamide–acrylic acid) and epoxidized natural rubber (ENR) in a dual ethylene glycol/water (EG/H₂O) solvent by one-pot thermal polymerization method, which can be served as an absorbent and an adhesive. The introduction of ENR provides a prominent improvement in the overall properties of hydrogels, including toughness and adhesion, due to its intrinsic nature. The hydrogels with chemical and physical dual crosslinks enable a better adsorption value of 113.2&#xa0;mg/g for methylene blue (MB), excellent adhesion for diversity substrates including natural rubber glove, glass culture dish, plastic, glass, and polytetrafluoroethylene (as high as 1700 N/m²), high swelling ratio (by 3156%), frost resistance, and solvent volatility resistance. The adsorption mechanism between hydrogel adsorbent and MB molecules mainly contains hydrogen bonding and electrostatic interaction. The experimental data can be more appropriately represented in pseudo-second-order kinetic and the Langmuir models, which reveal that the removal mechanisms are governed by chemical and monolayer adsorptions. As adhesive can be detached on demand, with no residual adhesive on the substrate and repeatable attachment and peel off, which would be conducive to practical applications in a particular scene. We anticipate that PAM-based functional hydrogels possess significant potential for various applications, including organic dye removal and water-soluble adhesive.</p> Graphical abstract <p></p>