This study focuses on the adsorption properties of activated carbon nanofibers (CNFs) fabricated by electrospinning polyacrylonitrile solutions dissolved in dimethylformamide, followed by heat treatment at high activation temperatures (700, 750, 800 degrees C). The samples were characterized by BET, SEM, and XRD. In addition, the adsorption energy distribution functions of CNFs were analyzed by using the generalized nonlinear regularization method. Comparative analysis of energy distribution functions provided significant information on the energetic and structural heterogeneities of CNFs. Furthermore, an investigation of adsorption equilibrium and kinetics of methylene blue (MB) and congo red (CR) revealed that the adsorption capacity and kinetics of MB are much higher and faster than that of CR on a given sample. Our experimental and theoretical results suggest that the CNFs used in this work may be widely used as an adsorbent.