Recent development of 2D materials opens a new way for the fabrication of low-dimensional structures with desired properties via controllable way. The most promising materials for nanoelectronics devices in the near future are graphene and different heterostructures based on them. Thus, it is necessary to create mechanisms of controlled modification of graphene electronic and magnetic properties to expand the application of graphene. Previous studies showed that this can be done by various techniques, for example, by using different substrates, mechanical deformations, chemical functionalization, introducing of various defects in graphene structure, and formation of heterostructures based on graphene. By combining different two-dimensional (like graphene, BN) and quasi-two-dimensional materials (for example, TMD) layered structures with van der Waals interlayer interaction can be obtained. In such materials the properties of individual components can be not only preserved but also new unique features can appear. Here an overview of theoretical and experimental results of effective way of modifying of physical and chemical properties of 2D structures via organic compounds and inorganic 2D materials functionalization were presented [1-4]. Features of the atomic structure and physical and chemical properties in a pair with possible ways for tuning of magnetic properties and shift the absorption spectra toward the visible range of the wavelength was performed. The work was supported by the Russian Science Foundation (No. 21-73-10238). [1] E. V. Sukhanova, D. G. Kvashnin, Z. I. Popov, Nanoscale 2020, 12, 23248. [2] E. V. Sukhanova, Z. I. Popov, D. G. Kvashnin, Jetp Lett. 2020, 111, 627. [3] M. Y. Lukianov, A. A. Rubekina, J. V. Bondareva, A. V. Sybachin, G. D. Diudbin, K. I. Maslakov, D. G. Kvashnin, O. G. Klimova-Korsmik, E. A. Shirshin, S. A. Evlashin, Nanomaterials 2023, 13, 1982. [4] A. N. Toksumakov, G. A. Ermolaev, M. K. Tatmyshevskiy, Y. A. Klishin, A. S. Slavich, I. V. Begichev, D. Stosic, D. I. Yakubovsky, D. G. Kvashnin, A. A. Vyshnevyy, A. V. Arsenin, V. S. Volkov, D. A. Ghazaryan, Commun Phys 2023, 6, 1.