Treatment of wastewater which containing organic dyes has attracted great attention in the last decades since organic dyes were produced in an increasing quantity. Hydrogel adsorbent, as a promising candidate for organic dye removal from aqueous solution, has been studied by many researchers in recent years. However, it’s still a challenge to create hydrogel adsorbent with high adsorption capacity and short contact time concurrently. Herein, we present a polyelectrolyte hydrogel adsorbent for anionic dyes removal which constructed by cationic monomer diallyldimethylammonium chloride (DADMAC) and acrylamide (AAm). Using calcium hydroxide nano-spherulites (CNS) as crosslinker, this physical hydrogel adsorbent showed a loosely crosslinked network structure. In optimal condition, the obtained P(AAm-DADMAC)/CNS hydrogel adsorbent showed a maximum adsorption capacity of 409 mg/g for methyl orange with a short contact time of 135 min. In addition, the adsorption process of this hydrogel adsorbent was well described by pseudo-first-order kinetic model and Langmuir adsorption isotherm model. Moreover, our P(AAm-DADMAC)/CNS hydrogel adsorbent also exhibited high adsorption capacities for other anionic dye, including Congo red (862 mg/g), Eriochrome black T (1139 mg/g) and methyl blue (722 mg/g). These results indicated that the P(AAm-DADMAC)/CNS hydrogel was a promising adsorbent material in wastewater treatment application.