In this Communication, we report MoO nanocomposites in which the near-infrared and visible light transmittance can be selectively modulated through the crystallinity. The MoO nanocomposites were fabricated by a hydrothermal method, and their optical properties were characterized by UV-Vis spectrometer. The obtained results proved the possibility to tune the nanocomposite's optical properties in the UV/Visible spectral region: crystalline MoO mainly regulates the near-infrared range (800-2600 nm), and amorphous MoO mainly changes the visible range from 350 nm to 800 nm and MoO , with semi-crystalline structures mainly modulating around 800-1000 nm. These kinds of optical modulations could be attributed to small polar absorption, free electron absorption and plasmon absorption according to different crystallinity. Our work may create new possibilities for future applications such as photochromism, photocatalysis, and electrochromism.