Being one type of the most abundant marine polysaccharides in nature, chitin has inert chemical properties and thus prolonged been hindered for high-value utilization. A mussel-inspired catecholic chemistry was found to be able to confer nature-derived mesoporous chitin aerogels with high and tunable surface activities. When further combining with their high porosity, high specific surface area, mechanical toughness and unique nanofibrous architecture, these catechol-activated chitin aerogels could be used as a unique supporting matrix to immobilize Ag nanoparticles. Besides the mild synthesis conditions and the merits inherited from pristine chitin, the resultant chitin-Ag hybrid aerogels further exhibited high catalytic activity, excellent recyclability, super solvent endurance and fast regeneration ability. Their high mechanic properties and porous structures also enabled a convenient membrane process to remove organic dyes from water. (C) 2017 Elsevier Inc. All rights reserved.