Analogous to Zn-rich primer for steel substrate, Al-rich primer is currently being investigated for their efficiency in protecting Aluminum based substrates. Various such primer systems were prepared with varying pigment size, with and without surface treatment. Electrochemical measurements such as open circuit potential, electrochemical impedance spectroscopy, and potentiostatic experiments were performed to obtain primer efficiency, such as throwing power and protection longevity. Data from electrochemical experiments will be used as boundary conditions and input parameters for computational modeling of the primer systems to investigate if results obtained from electrochemical measurements is complemented by computational results.