This study presents the preparation of membranes of polylactic acid (PLLA), polyacrylonitrile (PAN) and their corresponding membranes coated with polyaniline (PANI) for the adsorption of methylene blue (MB). Scanning electron microscopy micrographs reveal that all the membranes exhibit nanofibrous morphology. The adsorption capacity and the removal efficiency of the membranes are studied as a function of (initial adsorbate concentration, pH of the medium, temperature, contact time and adsorbent dosage). Coated membranes with PANI showed better adsorption performance and their DC conductivities were correlated to MB concentrations. Adsorption isotherms have also been performed and the adsorption process has been tested according to Langmuir and Freundlich models. The regeneration and reuse of the prepared membranes to re-adsorb MB were also investigated. The enhancement in adsorption performance and reusability of PANI-coated membranes in comparison with non-coated ones are fully discussed.