V1–xMoxO2thin films were fabricated by nanolamination of VO2/MoO3alternating layers using atomic layer deposition (ALD) process, in which tetrakis-dimethyl-amino vanadium(IV) [V(NMe2)4] and molybdenum hexacarbonyl(VI) [Mo(CO)6] were used as vanadium and molybdenum precursors, respectively. The dopant content of V1–xMoxO2films was controlled by adjusting MoO3cycle percentage (PMo) in ALD pulse sequence, which varied from 2 to 10%. Effects of PMoon V1–xMoxO2crystal structure, morphology, semiconductor-to-metal transition properties, and optical transmittance were studied. A linear reduction of phase transition temperature (Tc) by approximately −11 °C/cycle % Mo was observed for V1–xMoxO2films within PMo≤ 5%. Notably, dramatic enhanced luminous transmittance (Tlum= 63.8%) and solar modulation (ΔTsol= 23.5%) were observed for V1–xMoxO2film with PMo= 7%.