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An alginate gel bead composite adsorbent with polyethyleneimine (PEI) as a surface modifier and Eichhornia crassipes (EC) biochar, known as EC-alg/PEI-3, was added internally to the adsorb Cr(VI) from an aqueous environment. The functionalized gel beads were characterized using SEM, XPS, FTIR, and other techniques. The maximum adsorption capacities of EC-alg/PEI-3 were 714.3 mg g−1 at 10 °C and 769.2 mg g−1 at 25 °C. In the treatment of highly concentrated electroplating wastewater, EC-alg/PEI-3 can be dosed at 1.4 g L−1 to reduce the concentration of Cr(VI) to below 0.05 ppm. EC-alg/PEI-3 maintained a competitive adsorption capacity after six cycles. This spherical adsorbent material is easy to prepare, has a very high adsorption capacity, is environmentally friendly, and can be easily recycled. The EC-alg/PEI-3 gel beads are promising for the treatment of industrial wastewater.