Hydrophobically End-capped polyethylene oxide Urethane Resin(HEUR)-associating polymers, HEUR 35(8), HEUR 35 (12), and HEUR 35 (18), comprise a polyethylene oxide (PEO) having a molecular weight of 35,000 that is end capped with two C 8 H 17 , C 12 H 25 , and C 18 H 37 alkyl chains, respectively. These associating polymers were synthesized by condensation reactions with polyethylene oxides and alkyl isocyanates. The self-diffusion coefficients of HEUR-associating polymers were measured in aqueous solution by pulsed-gradient spin-echo (PGSE) nuclear magnetic resonance (NMR) spectroscopy. All polymers underwent a decrease in their mean diffusion coefficients as the concentration was increased. However, the dispersion of the diffusion coefficients, β, about the mean fluctuated with changes in concentration. The large dispersion at low concentrations of HEUR 35(8) and HEUR 35 (12) is related to the interaction between hydrophobic end groups, and the large dispersion at high concentrations of HEUR 35(18) is correlated with transient network formation. These results are valuable for predicting the associating mechanism of the large aggregates before and after their critical micelle concentration.