Display omitted •Green natural versatile adsorbent (efficiently remove Cr(VI), Pb(II) and dyes).•Higher adsorption performance under batch and fixed-bed condition.•Convenient for large scale application.•Excellent stability, reusability and convenient separation. Chitosan is highly suitable for removing metal ions and dyes from water; however, the sorption performance, stability and recycling are still critical issues in practical applications. Herein, polydopamine-modified-chitosan (CS-PDA) aerogels were synthesized through dopamine self-polymerization and glutaraldehyde cross-linking reactions to enhance the adsorption capacity and acid resistance of chitosan. The self-polymerization of dopamine and gelation of chitosan were accomplished simultaneously, simplifying the synthesis process of CS-PDA aerogels, which is meaningful for the popularization and industrial application of adsorbent. CS-PDA exhibited superior adsorption performances in the removal of Cr(VI), Pb(II) and organic dyes. Adsorption isotherms and kinetic data were well fitted by Langmuir and pseudo-second-order kinetic models. The maximum adsorption capacities of CS-PDA for Cr(VI) and Pb(II) were 374.4 and 441.2 mg g−1, respectively. After eight cycles, adsorption capacity of CS-PDA showed no obvious decline. These superiorities make CS-PDA a promising multifunctional adsorbent for the purification of metal ions and dyes.