The application of porous aerogels for dye adsorption has proven to be an effective approach in wastewater treatment. In this study, bio-cellulose aerogels from coconut fibrils were successfully developed via the formation of physically cross-linking cellulose with non-toxic binders (polyvinyl alcohol (PVA) and xanthan gum (XTG)) after a freeze-drying technique. The resulting cellulose aerogel demonstrated remarkably low density (27.59–47.76 g/cm3), high porosity (> 96.0%), a specific surface area of 518.01 m2/g, and a desorption average pore diameter distribution of 3.77 nm. These aerogels were tested for crystal violet (CV) and methyl orange (MO) adsorption to evaluate their effectiveness in treating dye-polluted water via various conditions such as contact time, pH values, initial concentrations, and temperature. The dye adsorption process reached equilibrium after approx. 30 mins and strictly followed pseudo-second-order and the Redlich-Peterson model. FT-IR and SEM-EDX analyses proved that the adsorption mechanism is primarily ascribed to the hydrogen bonding, electrostatic, π-π, and Vander Waals interactions between aerogel and dye molecules. The eco-friendly synthesis of recycled cellulose aerogels from coconut fibrils using green chemicals holds great promise for dye elimination.