Cyclic voltammetry and linear sweep voltammetry analyses were utilized to systematically investigate the electrochemical behavior of ZnSe as a function of the applied potential and pH. The impact of the applied potential and pH was correlated with the film composition. The ZnSe composition, including a stoichiometric composition (Zn:Se = 1:1), was controlled using the applied potential in aqueous alkaline electrolytes containing citrate, since the reduced difference of the reduction potentials between Zn and Se ions was due to the predominant Se electroactive species enabling the underpotential deposition of ZnSe. The morphology and crystallinity of the ZnSe thin films electrodeposited in the electrolytes at different pH were characterized by SEM and XRD analysis. The annealing temperature-dependent crystallinities of the ZnSe thin films were also analyzed. (C) 2016 The Electrochemical Society. All rights reserved.