The present study delves into the transformative effects of electrochemical oxidation on the hydrophobic-to-hydrophilic transition of carbon nanotube (CNT) sheets. The paper elucidates the inherent advantages of CNT sheets, such as high electrical conductivity and mechanical strength, and contrasts them with the limitations posed by their hydrophobic nature. A comprehensive investigation is conducted to demonstrate the efficacy of electrochemical oxidation treatment in modifying the surface properties of CNT sheets, thereby making them hydrophilic. The study reveals that the treatment not only is cost-effective and time-efficient compared to traditional plasma treatment methods but also results in a significant decrease in water contact angle. Mechanistic insights into the hydrophilic transition are provided, emphasizing the role of oxygen-containing functional groups introduced during the electrochemical oxidation process.