The effect of pH and salts concentration on the equilibrium swelling of the vermiculite/poly(2-acrylamido-2-methyl-1-propanesulfonic acid-co-acrylic acid) (VMT/P(AMPS-co-AA)) superabsorbent composite prepared by glow discharge electrolysis plasma (GDEP) were studied systematically. Factors influencing the adsorption of superabsorbent composite for cationic dyes such as pH, adsorption time, dye concentration were investigated in detail by batch experiments. Adsorption-desorption properties of materials were studied as well. The results showed that the superabsorbent composite has pH sensitivity, salt sensitivity, high water absorbency and adsorption capacity. The maximum equilibrium swelling ratio of the superabsorbent composite in distilled water is 822.4 g/g. The maximum adsorption capacities of the superabsorbent composite for Methylene blue (MB), Crystal violet (CV) and Malachite green (MG) are 2027.8, 2171.8 and 883.2 mg/g, respectively. The adsorption process of dyes follows the pseudo-second-order kinetic model with multi-step diffusion process at pH=6.5 and 25. In addition, VMT/P(AMPS-co-AM) hydrogel has certain adsorption-desorption performance, and can be also regenerated and reused.