Modification of membrane surface fabricated from bionanocellulose (BNC) carboxymethylcellulose (CMC) blend (BNC-CMC) with covalently bounded silicone layer was carried out in view of developing the novel, moist wound dressing material. The procedure was initiated with the reaction of aminopropyltriethoxysilane (APS) with carboxymethyl groups of CMC resulting with amide bound formation. The thickness of the silicone layer was further increased in the base-catalyzed polycondensation of silicone precursors: vinyltriethoxysilane (VES) or allyltrimethoxysilane (ATMS) initiated by N-(3-dimethylaminopropyl)-N'-ethylcarbodiimide hydrochloride (EDC). Surface modification was confirmed using various physicochemical methods such as FTIR, SEM, XPS and contact angle measurements. Swelling and drying tests confirmed that silicone-modified materials have considerable better water storage properties than the pristine BNC-CMC nanocomposite. The fabricated silicone modified BNC-CMC membranes are promising materials for wound dressing ensuring improved hydrobalance as the protective layer slows the evaporation of water.