Using polyvinyl alcohol (PVA) crosslinked with glutaric dialdehyde (c-PVA) as matrix and activated carbon (AC) or crosslinked polyacrylic acid (PAA) as the adsorptive constituent, large beads of c-PVA-AC and c-PVA-PAA composites were prepared via the sedimentation polymerization method. In this method, an aqueous solution of PVA, glutaric dialdehyde, and a catalyst for crosslinking (hydrochloric acid), containing activated carbon or the precursors of the crosslinked polyacrylic acid was injected dropwise with a syringe into hot mineral oil (about 80-90°C) located in a cylindrical reactor fit with a stirrer near its bottom. Partial gelation took place during the sedimentation process. This ensured that the particles arrived at the bottom of the column, where they were kept about 30-60 min to complete their polymerization, maintained their individuality without aggregation. The particle size was as large as about 3 mm. The adsorption characteristics of the two types of adsorbents were dependent on their AC or PAA content. Their adsorption capacity for four dyes was investigated. The c-PVA-AC and c-PVA-PAA had, at room temperature, saturation adsorption capacities as large as 84 and 104 mg/g for the basic Chrysoidin dye, and 70 and 72 mg/g for the basic Bismarck brown Y dye.