Pulsed field gradient NMR spectroscopy was used to investigate the association of toluene, chlorobenzene and benzyl alcohol with amino acid and dipeptide terminated polymerized surfactants (PS). The diffusion coefficient for each probe was measured in the presence and absence of the polymers and the mole fraction of bound probe molecules, f b , was calculated. For all solutions investigated, the probes associated more strongly with unpolymerized surfactant micelles than with corresponding PS. For example, the toluene f b values for association with sodium undecanoyl valinate micelles and the PS poly(sodium undecanoyl valinate) were 0.88 and 0.15, respectively. The relatively weak probe-polymer association was attributed to the polarity and fluidity of the polymers' hydrocarbon cores and to the fact that these PS have smaller aggregation numbers than the corresponding unpolymerized surfactant micelles.