A useful methodology is represented to functionalize polyacrylonitrile nanofibers by using humic acid as a makeup agent in electrospinning process. Both morphology and surface chemistry of polyacrylonitrile nanofiber mats were understood to be influenced by incorporation of humic acid into the structure. Physicochemical changes were evidenced by Fourier transform infrared spectroscopy, scanning electron microscope, and surface charge measurements. Unlike some anionic dyes (i.e., methyl orange, methyl red, and Congo red), there was an enhancement in crystal violet (a cationic dye) adsorption after incorporation of humic acid. The Langmuir model fitted well to crystal violet data, and monolayer adsorption capacity was calculated as 81.6 mg/g (r2 = 0.998).