In this study, linear polarization resistance (LPR) of pulse reverse electrodeposited graphene oxide (PREGO) coating is optimized by design of experiments approach (central composite design). Pulse current density (i), cathodic (Tc) and anodic (Ta) pulse durations, and total electrodeposition time (Tt) are selected as the substantial factors. The best prediction model proposes a definitive linear relation without any significant interaction of the LPR by analysis of variance. The desirable value of LPR was predicted equal to 5358 Ω cm2, obtaining at the pulse current density of 235.62 mA cm−2, Ta of 7.75 ms, Tc equal to 3.25 ms (f = 100 Hz), and Tt of approximately 225 s. Appearance of the XRD peaks at 25.11° and 27.18° and declining coating impedance up to 21 Ω cm2, as well as the elimination of functional groups at FT-IR spectra, are vividly promised the formation of sp2 domains in the PREGO coating.