In view of the simple and rapid conveniency of magnetic separation, magnetic nanocomposites had notably gained attention from researchers for environmental field applications. In this work, carboxylated magnetic multi-walled carbon nanotubes (c-MMWCNTs) and novel sulfonated MMWCNTs (s-MMWCNTs) were synthesized by a facile solvent-free direct doping method. Fourier transform infrared spectroscopy, X-ray diffraction, scanning electron microscope, energy dispersive X-ray, vibrating sample magnetometer, and point of zero charge analyses confirmed the successful doping of the Fe3O4 nanoparticles into the functionalized MWCNTs to form MMWCNTs. Besides, the bonding stabilities of both c-MMWCNTs and s-MMWCNTs were compared, and results showed that s-MMWCNTs possessed more substantial bonding stability than that of c-MMWCNTs with significantly less leaching amount of Fe3O4. The adsorption capacity of s-MMWCNTs was higher than that of c-MMWCNTs owing to the stronger electronegativity sulfonic group in s-MMWCNTs. Moreover, the reusability experiments proved that the adsorbent remained consistently excellent MB removal efficiency (R > 94%) even reused for twelve cycles of batch adsorption. The finding of the present work highlights the simple fabrication of novel s-MMWCNTs and its potential to be served as a promising and sustainable adsorbent for water remediation owing to its enhanced bonding stability, high adsorption performance, magnetic separability, and supreme recyclability.