In the present work, carbon nanotubes (CNT)/alginate composite adsorbent was prepared using combined method of magnetic field/electrospray. The effects of magnetic and electric fields on CNT orientation in the polymeric matrix of adsorbent, and consequently on the methylene blue adsorption were investigated. The adsorbents characteristics and adsorption performance of the six types samples were obtained using field-emission scanning electron microscopy (FE-SEM) and Ultraviolet-visible (UV-Vis) spectroscopy, respectively. The FE-SEM image observations indicated that under the setup’s operating condition, the magnetic field could partially orient the CNTs in the polymer matrix while the electrical field had a little effect. The obtained results clearly represented the positive effects of CNT orientation on enhancing the adsorption of methylene blue into the CNT/alginate composite adsorbents. The egg-box model in the CNT/alginate core-shell type beads could explain the adsorption performance of methylene blue solution onto the six types fabricated beads.