Tailoring of oxide chemistry on aluminum by means of low-pressure water and argon plasma surface modification was performed to influence the kinetics of the self-assembly process of octadecylphosphonic acid monolayers. The plasma-induced surface chemistry was studied by in situ FTIR reflection-absorption spectroscopy (IRRAS). Ex situ IRRAS and X-ray photoelectron spectroscopy were applied for the analysis of the adsorbed self-assembled monolayers. The plasma-induced variation of the hydroxide to oxide ratio led to different adsorption kinetics of the phosphonic acid from dilute ethanol solutions as measured by means of a quartz crystal microbalance. Water plasma treatment caused a significant increase in the density of surface hydroxyl groups in comparison to that of the argon-plasma-treated surface. The hydroxyl-rich surface led to significantly accelerated adsorption kinetics of the phosphonic acid with a time of monolayer formation of less than 1 min. On the contrary, decreasing the surface hydroxyl density slowed the adsorption kinetics.