A combinatorial method has been used to investigate the effects of anodic current density, and Mn(II) and H2SO4 concentrations on the electrochemical synthesis and characterization of electrolytic manganese dioxide (EMD). The combinatorial method involved rapid parallel and series electrochemical deposition of EMD from electrolytes with various Mn(II) (0.15-1.82 M) and H2SO4 (0.05-0.51 M) concentrations, at various anodic current densities (25-100 A m(-2)), onto individual 1 mm(2) titanium electrodes, in an overall array consisting of 64 electrodes. Electrode characterization was then by average plating voltage (recorded during deposition), and open circuit voltage and chronoamperometric discharge in 9 M KOH. The applicability and benefit of the method was demonstrated by identifying the conditions of 0.59 M Mn(II), 0.17 M H2SO4 and 62.5 A m(-2) anodic current density as leading to the best performing EMD. These are comparable with existing knowledge regarding the synthesis and electrochemical performance of EMD, demonstrating clearly the capabilities of the combinatorial method, and providing a starting point for future experimentation. An added benefit of the method in this work was the considerable time saved during experimentation.