Sol-gel/carbon nanotubes (CNTs) nano-composite films were electrochemically deposited by applying negative potential to a conducting substrate, i.e. indium tin oxide (ITO) and Ag grid printed on polyethylene terephthalate (PET). The deposition is driven by the local pH rise on the cathode that catalyzes the formation of sol-gel films. The latter serves as binder and entrapment for CNTs. The 10 deposition can be well manipulated by deposition potential and time, and the film can be selectively electrodeposited on the conductive parts of Ag grids printed on PET from an optimized dispersion. The thickness, transmittance, morphology and hydrophilicity of the films are characterized by profilometry, spectrophotometer, scanning electron microscopy (SEM) and water contact angle, respectively. It is further revealed that the electrodeposited sol-gel/CNTs composite films have non-linear optical properties 15 and exhibit pronounced antireflective performance (specular reflection < 0.5% over visible to long-wave IR range, allowing their potential applications as optical materials. Journal Name, [year], [vol], 00-00 | 5 65The composite films are hydrophilic, and can be selectively electrodeposited on conductive surfaces. Finally, we demonstrated that the electrodeposited sol-gel/CNT composite films show good non-linear optical properties and pronounced antireflection performance (blackness), which are mainly 70 attributed to the high content of CNTs in the films. This work suggests electrodeposition as a powerful method of preparing solgel/CNT composite films for optical applications.This work reports a method of electrodepositing sol-gel/CNT composite films. The deposition is highly selective to conductive surfaces, and the films show non-linear optical properties and excellent antireflection performance.