We have successfully prepared Congo Red-based polyurethane ionomers at our lab, and these ionomer structures have been proven by infrared (IR) spectra. For a dye-based polyurethane ionomer molecule solution, the surface tension was found to decrease, but the number-average particle size was found to increase with increasing concentration of Congo Red employed to prepare this ionomer molecule. Interestingly, the number-average particle size of dye-based polyurethane ionomer molecules decreases with increasing concentration of Congo Red in the presence of other dyes (i.e., Remajol Brilliant Blue R and Amaranth), as a result of Congo Red intramolecular interaction. It is important to point out that the addition of a fixed concentration of Amaranth to prepare Congo Red-based polyurethane ionomer molecules will significantly enhance the tensile strength but will decrease the elongation of this ionomer molecule.