X-ray diffraction technique was used to quantify change of cellulose crystallinity during refining. XRD data confirmed that fiber wall delamination was caused by the structural conversion of celluloses which occurred in a liquid medium during refining. The quantified crystallinity of celluloses in pulp fibers was closely associated with the change of fiber wall delamination, which was defined by measurement of fiber wall thickness. In particular, it was well recognized that low intensity beating showed a better response in the change of crystallinity than high intensity one. The decrease o cellulose crystallinity during refining considerably enhanced the improvement of interfiber bonding ability of a dried sheet.