The SERS (surface enhanced Raman spectroscopy) substrates based on nanocomposite porous films with gold nanoparticles (Au NPs) arrays were formed using the method of the pulsed laser deposition from the back low-energy flux of erosion torch particles on the glass substrate fixed at the target plain. The dependencies of porosity, and morphology of the surface of the film regions located near and far from the torch axis on the laser ablation regime, laser pulses energy density, their number, and argon pressure in the vacuum chamber, were ascertained. The Au NPs arrays with the controllable extinction spectra caused by the local surface plasmon resonance were prepared. The possibility of the formation of SERS substrates for the detection of the Rhodamine 6G molecules with the concentration 10−10 Mol/L with the enhancement factor 4·107 was shown.