Carbon nanowalls (CNWs) functionalization allows the tailoring of some of their properties after they have been synthesized. Herewith we report on post‐synthesis CNWs functionalization by plasma treatments. Radiofrequency plasmas generated in hydrogen, oxygen, nitrogen, tetrafluoroethane, and sulfur hexafluoride admixed to argon, were used. The changes of morphology, structure, chemical composition were determined by SEM, FTIR, Raman Spectroscopy, specifically for each gas mixture. The results point out to the surface erosion, the functional groups attachment, or to thin film coverage of CNWs material. Such processes strongly influence the material properties, as exemplified by the wettability: superhydrophilic or superhydrophobic surfaces are obtained starting from the same base CNWs material.