Polyurethane-urea anionomer dispersions with different stoichiometric DMPA/polyol and NCO/OH ratios were prepared from poly(oxypropylene)glycol, toluene diisocyanate (TDI), dimethylolpropionic acid (DMPA), and ethylenediamine (EDA). The dispersion-cast films were prepared and characterized by mechanical properties, dynamic mechanical analysis (DMA), and differential scanning calorimetry (DSC). Increasing the hard-segment content by either increasing the DMPA/polyol or the NCO/OH ratios affects the glass transition temperature (T-g) of the soft segments.