The present invention provides a method of manufacturing a highly functional surface-modified fibrous material with high added value, to which a novel functionality is imparted while making use of the characteristics inherent in the fibrous material, by modifying the surface of a natural fibrous material derived from an animal or a plant, or of a synthetic fiber; and a surface-modified fibrous material thereby obtained. The method of manufacturing a surface-modified fibrous material according to the invention includes attaching an inorganic material on the surface of a fibrous material by a sol-gel reaction, while allowing the fibrous material to move via an air stream. Preferably, an atmospheric-pressure low-temperature plasma is further applied to the surface of the fibrous material on the surface of which the inorganic material has been attached, while allowing the fibrous material to move via an air stream.