Hydrogen bonding in the hard segments of the synthesized montmorillonite/polyurethane nanocomposites of various hard segment ratios was found to decrease with the increasing amount of montmorillonite regardless of the hard segment ratios, but reached plateau values at 5 wt% montmorillonite concentration. The maximal reductions of the hydrogen bonding in the polyurethane nanocomposites ranged from 20 to 37%, depending on the hard segment ratios as compared to that in the pure polyurethane. The maximal strength and the elongation at break of the polyurethane nanocomposites increased dramatically as compared to that of pristine polyurethane, and the maximal values occurred at 1 wt% montmorillonite concentration. (C) 2001 Elsevier Science Ltd. All rights reserved.