Solution and adsorption properties of both charged and uncharged bottle-brush polymers have been investigated. The solution conformation and interactions in solution have been investigated by small-angle scattering techniques. The association of the bottle-brush polymers with anionic surfactants has also been studied. Surfactant binding isothermmeasurements,NMR, surface tensionmeasurements, aswell as SAXS, SANS and light scattering techniques were utilized for understanding the association behaviour in bulk solutions. The adsorption of the bottle-brush polymers onto oppositely charged surfaces has been explored using a battery of techniques, including reflectometry, ellipsometry, quartz crystal microbalance, and neutron reflectivity. The combination of these techniques allowed determination of adsorbedmass, layer thickness,water content, and structural changes occurring during layer formation. The adsorption ontomicawas found to be very different to that on silica, and an explanation for this was sought by employing a lattice mean-field theory. The model was able to reproduce a number of salient experimental features characterizing the adsorption of the bottle-brush polymers over a wide range of compositions, spanning fromuncharged bottle-brushes to linear polyelectrolytes. This allowed us to shed light on the importance of electrostatic surface properties and non-electrostatic surface-polymer affinity for the adsorption. The interactions between bottle-brush polymers and anionic surfactants in adsorbed layers have alsobeen elucidated using ellipsometry, neutron reflectivity and surface force measurements.