A majority of the reported electrografting of aryldiazonium salts result in the formation of covalently attached films with a limited surface coverage of below 5 nmol.cm(-2). Herein, we report the preparation of higher-thickness redox-active viologen-grafted electrodes from the electro-reduction of viologen phenyl diazonium salts, by either cyclic voltammetric (CV) sweeps or electrolysis using a fixed potential. Both of the methodologies were successfully applied for various conductive surfaces, including glassy carbon (GC), gold disc, indium tin oxide glass, mesoporous TiO2 electrodes, and 3D compacted carbon fibers. A robust maximal viologen coverage, Gamma(viologen) = 9.5 nmol.cm(-2), was achieved on a GC electrode by CV electroreduction. Electroreduction held at a fixed potential at E-appl.. = -0.3 V can fabricate viologen-grafted electrodes with Gamma(viologen) in the range of 0-37 nmol.cm(-2) in a controllable way, by simply adjusting the electrodeposition time t(appl.). Time-dependent Gamma(viologen) were found to be 10 nmol.cm(-2)@2 min, 20 nmol.cm(-2)@4.2 min, and 30 nmol.cm(-2)@7 min. Furthermore, a TiO2 electrode coupled with Gamma(viologen) of 140 nmol.cm(-2) exhibited electrochromic performance, with the color changing from pale yellow to blue and red brown.