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Transparent conductive oxides such as indium tin oxide (ITO) substrates are commonly employed as prime materials for optoelectronic applications. Enhancement in functions of such devices often compels stable and robust modification of the ITO substrate to improve its interfacial charge transfer characteristics. Thereby, in this work, naphthyl modifier multilayer films are fabricated on ITO substrate using conventional electrochemical reduction of 1-naphthyl diazonium salts (NAPH-D) via altering its concentration ranging from 2 mM to 12 mM with a step size of 2. Surface coverage was significantly tuned by varying NAPH-D concentration, keeping other parameters such as the number of scans and scan rate constant. For lower concentrations (2 mM), the molecular thickness ∼6 nm was obtained, whereas higher concentrations (12 mM) produced around 15–18 nm thickness. Atomic force microscopy (AFM), cyclic voltammetry, and electrochemical impedance spectroscopy (EIS) in the presence of a ferrocene redox probe also supports the formation of well packed molecular film grown on the ITO surface. Further, the wettability property of the grafted naphthyl film was investigated at different surface coverages and correlated with charge transfer resistance (RCt) obtained from EIS studies. [ABSTRACT FROM AUTHOR]