The interaction between polyelectrolyte grafted fullerenes and surfactants was elucidated using a dual polarization interferometer (DPI). The deposition of poly(2-(dimethylamino)ethyl methacrylate) (PDMA(50)-b-C-60) at pH 6 on the surface of silicon oxynitride induced by electrostatic interaction between charged PDMA segments and negatively charged surface revealed an adsorption thickness similar to the diameter of a fullerene molecule. A second deposition of poly(acrylic acid)-block-C-60 (PAA(83)-b-C-60) on adsorbed PDMA(50)-b-C-60 at pH 6 was facilitated by electrostatic interaction between negatively and positively charged PAA and PDMA segments, respectively. A monolayer of PAA(83)-b-C-60 adsorbed on PDMA(50)-b-C-60 layer yielded a thickness twice the diameter of C-60 molecules. As a comparison, a two end-capped C-60-PAA(83)-C-60 was examined, where the packing thickness and mass were smaller than the monocapped system due to steric hindrance effect of fullerene molecules. The adsorption of two nonionic surfactants (i.e., polyoxyethylene 9 lauryl ether (Brij 76) and octyl phenol ethoxylate (Triton X-100 or TX 100)) on the adsorbed PDMA-C-60 layer was examined. Both Brij 76 and TX 100 interacted with the PDMA-C-60 layer. For TX 100, the interaction was promoted by pi-pi interaction between the C-60 headgroup and phenyl ring of the surfactant. Beyond the critical micellar concentration of TX 100, the adsorption was greatly reduced. The concentration effect of first layer PDMA-C-60 was evaluated, where the PDMA-C-60 molecules adsorbed on the chip at higher density, resulting in a larger layer thickness. The densely packed fullerene headgroup hindered the penetration of TX 100 aromatic ring into the first layer.