A novel CO2 laser additive manufacturing technique is reported in this paper for depositing transparent TiO2 films on quartz substrates using anatase TiO2 nanoparticles (NPs). Single- and double-layers of TiO2 films were prepared in two stages: (i) wet deposition using the spin-coating technique, and (ii) laser-assisted both drying of the wet layer and then sintering of the dried NPs to form a film. A theoretical model is presented to select and optimize the laser processing parameters. Scanning electron microscopy (SEM) revealed that the laser heating induces necking and coalescence of TiO2 NPs without cracking the sintered films or damaging the quartz substrate. An anti-reflection coating (ARC) model is utilized to select the film material and film thickness, aiming to reduce the reflectance and enhance the transmittance at certain wavelengths. UV/Vis spectrophotometry showed transmittance above ∼90% in the visible (Vis) range. The effect of laser power on the enhancement of transmittance is presented in this paper. Different concentrations of TiO2 NPs were used to optimize the film thickness. Single layer (∼110nm thick) and double layer films of the same total thickness as the single layer were analyzed to infer the effects of interface on the transmittance of TiO2 films. The transmittance of the single layer is higher, same as that of the double layer. Therefore, the difference in the transmittance of the single- and double-layer may be due to the effect of interface. The optical properties of the anti-reflection TiO2 coating in the UV–Vis ranges were investigated. X-ray diffraction (XRD) analysis showed that the thickness affects the crystallinity of the sintered TiO2 films.