The organic-silicon films, polytetrafluorethylene (PTFE) films and its composite films with copper have been fabricated from an active gas phase by pulse laser dispersion from initial powder species. The features of all films obtained were studied with the application of attenuated total reﬂection-Fourier transform infrared (ATR-FTIR) spectroscopy. Our results suggest that the wavelength of laser radiation impact a strong effect on the molecular structure of all films. Specifically, the peaks corresponding to the detachment of C-H bonds in the organic-silicon films and its Cu doped films at a laser wavelength of 532 nm and the destruction of the Si-O-Si groups at 266 nm due to the ultraviolet radiation have been observed. Interestingly, the concentration of Si-С6Н5 groups relative increases with a decremental of the wavelength of laser radiation. In addition, the PTFE films formed at a laser wavelength of 355 nm presented a lower order degree and high amorphous phase, while PTFE-Cu composite films at laser wavelength 266 nm exhibited enhanced crystallinity due to the presence of copper species, wherein being served as nucleation centers. Remarkably, the wavelengths of laser radiation nearly play no effect on the orderness of PTFE-Cu composite films.