Lateral and normal forces between a surface-bound, brushlike copolymer, poly(ethylenimine)-graft-poly(ethylene glycol) (PEI-g-PEG), and a silica colloidal probe were investigated with atomic force microscopy (AFM) and related to the relative mass of the solvent absorbed within the polymer as measured with the quartz crystal microbalance. PEI-g-PEG was adsorbed onto an oxide-passivated silicon wafer through its exposure to physiologically buffered solutions of the polymer. Frictional forces were measured between the colloidal probe and the substrate by AFM as the polarity of the solvent was systematically varied. Reduced friction forces and greater film thicknesses were encountered under solvents of higher polarity, which are attributed to the extended conformation of the brushlike copolymer under these conditions. Lateral and normal forces detected between the colloidal probe and this surface-bound PEI-g-PEG were found to be similar under certain solvent conditions to those measured for poly(L-lysine)-graft-poly(ethylene glycol), a brushlike copolymer with a different molecular architecture. To this end, friction force studies of both symmetric and asymmetric PEI-g-PEG-coated interfaces served to identify the contributions of conformational and bridging effects in the observed tribological behavior.