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The paper presents the preparation and characterization of novel composite materials based on microcrystalline cellulose (MCC) with silver nanoparticles (Ag NPs) in powder and gel forms. We use a promising synthetic conception to form the novel composite biomaterials. At first MCC was modified with colloidal solution of Ag NPs in isopropyl alcohol prepared via metal vapor synthesis. Then Ag-containing MCC powder was used as precursor for further preparation of the gels. The hydrogels were prepared by dissolving pristine MCC and MCC-based composite at low temperatures in aqueous alkali solution and gelation at elevated temperature. To prepare aerogels the drying in supercritical carbon dioxide was implemented. The as-prepared cellulose composites were characterized in terms of morphology, structure, and phase composition. Since many functional properties, including biological activity, in metal-composites are determined by the nature of the metal-to-polymer matrix interaction, the electronic state of the metal was carefully studied. The studied cellulose-based materials containing biologically active Ag NPs may be of interest for use as wound healing or water-purification materials.