It is known that a material’s volume and the surface structuring by the nanoparticles causes a significant change in the material’s basic properties. In this aspect, the structuration of the surface of semiconductors is of interest, because their wide potential application in optoelectronics can extend the products’ transparency, hardness, wettability, and other important parameters. This paper presents possible methods for the surface modification of zinc selenide and zinc sulfide when carbon nanotubes are deposited on the surface by the application of the laser-oriented technique. It also shows changes of the spectral, mechanical, and wetting characteristics of the considered materials. Using the molecular dynamic simulations, the possible process of the carbon nanotubes penetration into the considered surfaces is presented. The simulation results are partially supported by the obtained experimental data.