Herein, we report cyclodextrins (CDs)-modified regenerated cellulose nanofibers (CDs/RCNFs) as green adsorbents for the removal of toluene from wastewater. Two different methods, namely, physical mixing and chemical grafting, were opted to combine the CDs with RCNFs. The CDs with three different kinds such as alpha-, beta-, and gamma were employed. Initially, various electrospinning parameters were optimized to obtain the better morphology of CDs/RCNFs. Scanning electron microscopy (SEM) results confirmed the good surface morphology of CDs/RCNFs. The effective dispersion and successful chemical modification of RCNFs with CDs were acknowledged by SEM, X-ray photoemission spectroscopy (XPS) and Fourier transform infrared spectroscopy (FT-IR) analyses. The usefulness of the prepared materials was realized from the higher adsorption rate of toluene. It was found that the chemically modified RCNFs with gamma-CDs have a better toluene adsorption rate of 82% after only 180 min. (C) 2016 Taiwan Institute of Chemical Engineers. Published by Elsevier B.V. All rights reserved.