A wide range of chemical reagents are capable of producing a satisfactory crease-resisting finish for cellulosic fabrics and are currently available on the market. However, these agents do not work as efficiently on linen relative to cotton or rayon. Untreated linen controls and samples treated with a N-methylol reagent were investigated for physical and chemical changes, and an attempt was made to quantify the crosslinking bonds formed and assess other changes in the treated fabrics using Fourier transform infrared spectroscopy (FTIR) and visible and near-infrared spectroscopy (NIR). The results were compared with nitrogen analysis data, crease-recovery angle measurements, and abrasion-resistance tests in an attempt to assess the effectiveness of the treatment relative to the responses of the instrumental techniques. This study shows correlations between the visible and NIR and FTIR spectra and the crease-recovery angle and abrasion resistance. The study also indicates that FTIR may be useful in assessing the crosslinking bonding changes associated with the dimethylol urea treatment of linen to achieve improved crease recovery.