Cellulose nanocrystals (CNCs) is an exciting class of sustainable and carbohydrate material, which has great potential applications in molecular adsorption. However, the complex preparation process and limited adsorption capacity of CNCs hinder its commercial application. In this study, we design a novel functional cellulose nanocrystals-based adsorbent by an ingenious mixing of lignin-containing cellulose nanocrystals (LCNCs), sodium alginate (SA), and calcium chloride solution. Benefiting from the sulfonate groups of lignin, carboxyl groups of SA, the maximum adsorptive capability of LCNCs/SA beads for methylene blue was found to be 1181 mg g-1, which was significantly higher than previously reported biomass-based adsorbents. More importantly, LCNCs/SA beads can be reused several times. This strategy can not only improve the adsorption performance of CNCs-based materials, but also simplify the production technology of CNCs, which greatly promote the commercial application of CNCs materials.