The interaction of polyvinylpyrrolidone (PVP) with an anionic surfactant (sodium dodecyl sulfate, SDS), a nonionic surfactant (pentaethylene glycol monodecyl ether, C10E5), and a zwitterionic surfactant (lauryl amido propyl betaine, LAPB) has been investigated by means of pulsed gradient spin-echo NMR (FT-PGSE NMR), allowing self-diffusion coefficients to be determined. The results confirm the strong interaction prevailing in the PVP/SDS system, whereas no association has been observed in the PVP/C10E5 and PVP/LAPB systems. Mixing PVP with two surfactants, namely SDS and C10E5 or SDS and LAPB, results in the formation of ternary aggregates between the polymer and the mixed micelles.