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VMoO thin films were fabricated by nanolamination of VO/MoO alternating layers using atomic layer deposition (ALD) process, in which tetrakis-dimethyl-amino vanadium(IV) [V(NMe)] and molybdenum hexacarbonyl(VI) [Mo(CO)] were used as vanadium and molybdenum precursors, respectively. The dopant content of VMoO films was controlled by adjusting MoO cycle percentage (P) in ALD pulse sequence, which varied from 2 to 10%. Effects of P on VMoO crystal structure, morphology, semiconductor-to-metal transition properties, and optical transmittance were studied. A linear reduction of phase transition temperature (T) by approximately -11 °C/cycle % Mo was observed for VMoO films within P ≤ 5%. Notably, dramatic enhanced luminous transmittance (T = 63.8%) and solar modulation (ΔT = 23.5%) were observed for VMoO film with P = 7%.