This work explores the association of a pegylated lipid (DSPE-PEG) with different anionic and zwitterionic surfactants (pseudo-binary and pseudo-ternary polymer+ surfactant mixtures), and the adsorption of the polymer + surfactant aggregates onto negatively charged surfaces, with a surface charge density similar to that existing on the damaged hair epicuticle. Dynamic light scattering and zeta potential measurements shows that, in solution, the polymer + surfactant association results from an intricate balance between electrostatic and hydrophobic interactions, which leads to the formation of at least two different types of micellar-like polymer + surfactant aggregates. The structure and physicochemical properties of such aggregates were found strongly dependent on the specific nature and concentration of the surfactant. The adsorption of the polymer + surfactant aggregates onto negatively charged surface was studied using a set of surface-sensitive techniques (quartz crystal microbalance with dissipation monitoring, ellipsometry and Atomic Force Microscopy), which allows obtaining information about the adsorbed amount, the water content of the layers and the topography of the obtained films. Ion-dipole interactions between the negative charges of the surface and the oxyethylene groups of the polymer + surfactant aggregates appear as the main driving force of the deposition process. This is strongly dependent on the surfactant nature and its concentration, with the impact of the latter on the adsorption being especially critical when anionic surfactant are incorporated within the aggregates. This study opens important perspectives for modulating the deposition of a poorly interacting polymer onto negatively charged surfaces, which can impact in the fabrication on different aspects with technological and industrial interest.