The dissertation is devoted to the development and realization of the scientific concept of obtaining water-repellent thin-layer coatings for paper protection from unbleached cellulose based on of silicon-organic domestic products with various functional groups near the silicon atom able to chemical with its ingredients. It has been established that the main factors which can contribute to the increase of the level of consumer properties of paper can be its composition and structure, the reactivity of the surface, the use of siloxanes, which increase the stability of the material to the effect of moisture and mechanical strength. Using the methods of IR spectroscopy it was estimated the amount and strength of the O−H, C – H bonds and the adsorbed water in the paper composition. Hydroxyl groups are the most active groups of paper in terms of energy. Changing the parameters of the characteristic absorption bands of the valence vibrations of ON-groups evaluated the reactivity of the paper with respect to siloxanes with different functional groups and established the possibility of interaction of the EN–70 paper with silicone compounds with the participation of ON-groups. Complex researches of the processes of interaction between silicates with ≡Si-OK, ≡Si-OH, ≡Si-OС2Н5 bonds with cellulosic materials were conducted and the ways of their realization have been carried out in order to provide efficient and reliable protection of this materials. Taking into account the peculiarities of the composition and structure of the paper, schemes of barrier protective coatings on the basis of siloxanes with reactive groups ≡Si–H, ≡Si – OH, ≡Si – OS2H5 and metal-containing (Cu, Zn) organosilicates were developed. Were determined the optimal concentrations of the preparats (1.0–2.0 wt.%) and an ecologically safe way for their use in the form of water-soluble ammonia complexes. Schemes for the preparation of two-layer coatings with the use of potassium methyl siliconate and methyl silicates of copper and zinc as a biocide substrate-adhesive or ethyl silicate hydrolyzate for regulated surface shielding as well as polyalkylhydride siloxanes as an external layer were proposed. The commodity evaluation of paper with developed modified and two-layer silicone coatings in comparison with industrial silicone products was made. The efficiency of the use of silicone products on unbleached pulp paper by the indices of the wetting angle and the degree of screening of the surface growing in sequence: coatings based on industrial silicone products (ϴ = 84.4 °, X = 70.9%) < modified coatings (ϴ = 92,0 °, X = 81.8%) < two-layer coatings (ϴ = 93.7 °, X = 84.1%). High efficiency to achieve maximum strength is occupied by coatings based on modified polyethylhydridsiloxanes, as well as two-layer GETS / PMGS. The efficiency of application of the developed coatings for the protection of the paper from the complex effect of atmospheric factors was evaluated. By the degree of destructive action on paper with siloxane coatings (ϴ, X, mechanical strength) wet environments are located: water vapor <water vapor and microscopic mushrooms <water vapor and salt mist. It has been determined that the maximum limit of values of the marginal angle of wetting of cellulosic materials with protective coatings can be 94–104○. The action of liquid water is accompanied by minimal (ϴ = 104 °, X = 98%), and dew and frost − by maximum hydrophilization of the surface of the protected paper. The wettability for the modified and two-layer coatings at the final stage of testing is: is 86 - 93 °, the tensile strength is 51.6-58.0% (against 60 ° and 7.1%, respectively, in uncoated paper), the screening rate is X = 73.4-83.1%. Residual strength of cellulosic materials after the influence of destructive factors can reach 111% of the initial value when using modified polyalkylhydride siloxanes and double layer coatings with ethyl silicate hydrolyzates. The results of scientific researches were realized in the production conditions of the state enterprise «Coloran» of NAS of Ukraine and LLC «Polygon», the industrial testing of the developed thin-layer coatings for paper was carried out, the efficiency of their use was proved, as evidenced by the acts of implementation. The novelty of technical solutions is protected by 3 patents of Ukraine for utility model.