Contact angle relaxation of partially wetting drops was studied on native and base hydrolyzed pyromellitic dianhydride (PMDA)-4,4'-oxydianiline (ODA) polyimide surfaces as a function of wetting liquid pH. Upon base hydrolysis, followed by acid neutralization, carboxylic acid groups are formed on the native polyimide surface. The areal density of incipient carboxylic acid groups is proportional to base hydrolysis time. Wetting kinetics were examined on polyimide surfaces as a function of hydrolysis time and wetting liquid pH using the molecular-kinetic theoretical approach. The results of parametric fitting of experimental contact angle relaxation data using the molecular-kinetic approach indicate that the kinetics and thermodynamics of wetting were nearly invariant when using a pH 2 probe liquid for native compared to hydrolyzed surfaces. In contrast, the kinetics and thermodynamics of wetting using a pH 11 probe liquid exhibited large differences based on the extent of modification and ionization of the surface. The differences in kinetics appear to be due to a lesser interaction of the pH 11 probe liquid with modified surfaces.