AbstractCellulose is the Earth’s most abundant biopolymer. Exploiting its environmentally friendly attributes such as biodegradability, renewability, and high specific strength properties are limited by our inability to isolate them from the secondary cell wall in an economical manner. Intermolecular and intramolecular hydrogen bonding between the cellulose chains is the major force one needs to overcome in order to isolate the cellulose chain in its microfibrillar form. This paper describes how a hydrogen bond-specific enzyme disrupts the crystallinity of the cellulose, bringing about internal defibrillation within the cell wall. Bleached kraft softwood pulp was treated with a fungus (OS1) isolated from elm tree infected with Dutch elm disease. FT-IR spectral analysis indicated a significant reduction in the density of intermolecular and intramolecular hydrogen bonding within the fiber. X-ray spectrometry indicated a reduction in the crystallinity. The isolated nano-cellulose fibers also exhibited better mechanical strength compared to those isolated through conventional methods. The structural disorder created in the crystalline region in the plant cell wall by hydrogen bond-specific enzymes is a key step forward in the isolation of cellulose at its microfibrillar level.