A comprehensive understanding of chemical interactions at the surface of hair represents an important area of research within the cosmetic industry and is essential to obtain new products that exhibit both performance and sustainability. This paper aims at contributing to this research by applying a combination of surface techniques (neutron reflectometry, quartz-crystal microbalance and atomic force microscopy) to study adsorption of surface active ingredients onto hair-mimetic surfaces. The surface of hair is not homogeneous due to chemical and physical damage, and this work focuses on partly damaged hair models, in which both hydrophobic and charged moieties are present. Examples of such mixed-surface models are rare in the literature, despite the interest in the topic. The studied actives were an anionic surfactant (sodium dodecyl sulphate, SDS) and a natural polysaccharide (chitosan) of two different molecular weights, to represent soluble polymer-surfactant associations of cosmetic interest in hair-care rinsing applications. The effect of the concentration of SDS, the molecular weight of chitosan, and the order in which SDS and chitosan are introduced are studied, and compared to totally hydrophobic and totally hydrophilic surfaces. Results show that SDS can interact with the hydrophobic portions of the mixed surface, and its adsorption increases if associated with chitosan. Interestingly, differences have been found in the adsorption behaviour of chitosan depending on its chain size. Both types can deposit onto the surface, but when SDS is added, the lower molecular weight chitosan keeps its extended conformation in a ca. 70 Å thick layer, while the higher molecular weight chitosan collapses to form a layer of about 30 Å. This knowledge opens the door to developing hair-care formulations with improved performance and sustainability.