Chlorine doped ZnO thin films were grown by metal-organic chemical vapour deposition (MOCVD) on sapphire and fused silica substrates. Chlorine is incorporated by substitution of oxygen and acts as a donor, leading to an increase of electron concentration. Transport properties were studied for ZnO thin films with different chlorine content. Hall effect measurements show an increase of electron carrier concentration and a decrease of electron mobility upon increasing the amount of chlorine incorporated in ZnO. The lowest resistivity ρ = 3.6 × 10 − 3 Ω cm was obtained for layers deposited on sapphire substrate. UV–VIS–NIR spectroscopy has been used for the study of optical properties. For all samples, the optical transmittance in the visible range is greater than 80%. First principles computations were applied in order to examine the change in the band gap of ZnO with Cl doping.