In this study, we designed a novel hydrogel composite membrane based on the combination of polyvinyl alcohol (PVA), agar, and maltodextrin through a facile solution‐casting router. From Fourier‐transform infrared spectroscopy, contact angle, scanning electron microscopy, and swelling analyses, the formation of hydrogen bonds between surface functional groups of PVA, agar, and maltodextrin was confirmed. As a result, the PVA/agar/maltodextrin membranes exhibited a more hydrophobic nature compared with pure PVA. The thermal stability and integrity of such obtained composite membranes were also elucidated by the evaluation of thermogravimetric analysis and mechanical behavior. Besides, the composite membrane exhibited high selective adsorption for cationic dyes, namely 20.2 mg g−1 for methylene blue and 19.17 mg g−1 for crystal violet at initial dye concentration of 100 mg/L, an adsorbent dosage of 0.1 g, contact time of 180 min, and solution pH 7, while anionic dyes such as congo red and methyl orange are approximately zero. The adsorption kinetics and isotherm of the as‐prepared composite membranes were well fitted to the pseudo‐second‐order and Temkin model. The effect of factors, including contact time, solution pH, PVA content, and initial dye concentration on the adsorption capacity of the as‐prepared composite membrane was also investigated in detail. © 2019 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2019, 137, 48904.

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