A simple and novel method, self-assembly of nanocellulose and nanochitin, was developed to produce high-efficiency and versatile biohybrid hydrogel (BHH) and aerogel (BHA) for water purification. The self-assembly process was driven by the electrostatic force between one-dimensional (1D) negatively charged TEMPOoxidized cellulose nanofiber (TOCNF) and positively charged partly deacetylated chitin nanofiber (PDChNF). The self-assembly process was performed at room temperature and without adding any crosslinking agents throughout the process. This results in the threedimensional (3D) BHH that physically cross-linked via both electrostatic interactions and hydrogen bonding between TOCNF and PDChNF. The obtained BHA from lyophilized BHH exhibited a highly porous interconnected structure with a specific surface area of 54 m 2 •g −1 , which assures the availability of its internal active site for the adsorption of toxic metalloid ions and organic pollutants. Consequently, the BHA displayed super-high adsorption capacities of 217 mg•g −1 for As(III) under the neutral pH conditions and 531 mg•g −1 for methylene blue (MB) under an alkaline aqueous condition with rapid adsorption kinetics, in sharp contrast to conventional biobased adsorbents. Moreover, the BHA is reusable, which still exhibited a high MB adsorption capacity of 505 mg•g −1 even after five successive adsorption−desorption cycles. This versatile BHA produced via a facile preparation strategy is proven to be a promising renewable adsorbent for water purification, offering simple and green alternatives to the conventional adsorbent from synthetic polymers.