Herein, fabrication of a functionalized graphene aerogel (f-GA) from a biomass (pear fruit)-derived graphene aerogel (GA) is described. Functionalization showed a prominent effect that results in the improved adsorption capacity of f-GA compared to GA, and even better (∼more than double) than commercially available activated carbon (AC). f-GA has been studied for the removal of three different model pollutant dyes, namely crystal violet (CV), methylene blue (MB), rhodamine B (RhB) and their mixtures, along with it also being used for dye removal from unknown real industrial samples. Moreover, a detailed comparative analysis showed the adsorption capacity of f-GA towards CV, MB, and RhB has been improved up to ∼6, ∼7, and ∼10 times, respectively, compared to that of control GA. The recyclability of f-GA was also tested: it works for five cycles without losing its apparent performance.