The combined thin-layer protective coating for cellulose-containing materials includes a biocidal sublayer-adhesive composed of potassium methylsiliconate and an amino complex of copper and zinc methyl silicates, along with a basic protective layer of polyalkylhydridesiloxanes as the outer coating was studied. The synthesis of copper and zinc methyl silicates was carried out by reacting potassium methylsiliconate with copper sulfate and zinc chloride as fungicidal agents. An environmentally safe method for using copper and zinc methylsilicates through water-soluble ammonia complexes was suggested. The formation of chemical bonds between silanol groups and copper-zinc ions was demonstrated using IR spectroscopy. The use of two-layer organosilicon coatings has been substantiated to enhance moisture resistance and mold protection. The developed coatings can increase the hydrophobicity of the paper surface by up to 28.3% and reduce the hygroscopicity of paper by up to 20% compared to basic organosilicon products. Fungicidal properties and the ability to inhibit the development of mold are found on paper coated with adhesive sublayer from aqueous solution of the amino complex of copper and zinc methyl silicates and potassium methylsiliconate in a concentration of at least 1.5 and 2.0 wt.%, respectively.