In this study, a new type of silica-cellulose hybrid aerogel was synthesized through a green and facile chemical cross-linking process. In a first step, dendritic fibrous nanostructured (colloidal) silica particles (DFNS) were prepared by a simple hydrothermal technique. Then, the surface of DFNS particles was functionalized with amine groups using 3-aminopropyltriethoxysilane to produce DFNS-NH2. In a second step, bifunctional hairy nanocellulose (BHNC) particles were functionalized with both aldehyde and carboxylic groups. The aldehyde groups of BHNC and the amine groups of DFNS-NH2 chemically reacted through a Schiff base reaction to form a hybrid hydrogel nanocomposite. Therefore, no external cross-linker is required in the synthesis. This hybrid aerogel is very lightweight and highly porous with a density of 0.107 g mL-1 and a porosity of 93.0 ± 0.4%. It has a large surface area of 350 m2 g-1, a large pore volume of 0.23 cm3 g-1, and a small pore size of 3.9 nm. The developed aerogel contains both positively and negatively charged functional groups and is a highly efficient substrate for dye adsorption from water, for both cationic and anionic organic dyes. These aerogels were found to have an outstanding adsorption capacity toward methylene blue (MB) as a cationic dye and methyl orange (MO) as an anionic dye. The results show that the aerogels can adsorb MB and MO with a capacity of 270 and 300 mg dye/g adsorbent, respectively.