Removal of dyes through adsorption from wastewater has gained substantial interest in recent years, especially in development of hydrogel based adsorbents, owing to their easy use and economical nature. The aim of the present study was to design a super-adsorbent hydrogel based on sodium styrenesulfonate (NaSS) monomer for removal of dyes like methylene blue (MB). NaSS displays both an aromatic ring and strongly ionic group in its monomer structure that can enhance adsorption capacity. Poly(sodium styrenesulfonate-co-dimethylacrylamide) hydrogels were prepared by solution free radical polymerization using gelatin methacryloyl (GelMA) as crosslinker, creating a highly porous, three-dimensionally crosslinked polymer network contributing to higher swelling ratios of up to 27,500%. These super-adsorbent hydrogels exhibited high adsorption capacity of 1270 mg/g for MB adsorption with above 98% removal efficiency. This is the first report for such a high adsorption capacity for dye absorbance for NaSS-based hydrogels. Additionally, the adsorption kinetics using a pseudo-first-order and the Freundlich adsorption isotherm models for multilayer, heterogeneous adsorption processes has been reported. The adsorbents’ reusability was confirmed through 4 repeated cycles of desorption-adsorption. The results discussed herein illustrate that NaSS based chemistries can be used as an efficient option for removal of organic dyes from contaminated wastewater.