Silk sericin (SS) has been fabricated into beads using a 1 M LiCl/DMSO solvent and utilized as a heavy metal adsorbent. Among the various heavy metals, we targeted Cr(VI) for adsorption using SS beads and found that its adsorption depended on the coagulant used for the fabrication of the SS beads. When methanol was used as a coagulant, the beads had a better adsorption capacity than when ethanol was used except at pH 1. The adsorption behavior of Cr(VI) on the SS beads followed the BET isotherm. The maximum adsorption capacity was 33.76 mg/g at pH 2. The adsorption of Cr(VI) was confirmed by FT-IR and EDS analyses. Finally, the desorption was carried out using NaOH solution, and it was found that 73.19% of the adsorbed Cr(VI) could be detached.