In this study, zinc oxide nanoparticles (ZnO NPs) were biosynthesized with the use of an extract derived from seaweed (Sargassum sp.) and used as a sorbent for the removal of Cr(III) ions from wastewater. The biosorption properties of the seaweed itself as well as of the post-extraction residue were investigated for comparison. ZnO NPs were characterized with UV−vis, ICP-OES, FTIR, XRD, and SEM techniques. The sorption capacity of the (bio)sorbents was investigated as a function of contact time at different pH values and initial concentrations of metal ions. Sorption kinetics and isotherms were studied in order to comprehend the sorption nature and mechanism. The sorption kinetic data were well-fitted with the pseudo-second-order model, and the highest sorption capacity was calculated for ZnO NPs (137 mg/g), whereas those calculated for Sargassum sp. (82.0 mg/g) and the post-extraction residue (81.3 mg/g) were comparable (at pH 5 and 300 mg of Cr(III) ions/L). The adsorption isotherms for all sorbents were well described using the Langmuir model. According to these findings, ZnO NPs were superior to the sorption properties of the tested biosorbents and can be used as a potential sorbent for the removal of metal ions from wastewater. Renewable seaweed biomass can be used for the sustainable biosynthesis of nanoparticles used for environmental protection.