Most modern electrochemical and photoelectrochemical devices (e.g., solar cells, photoelectrochemical cells, fuel cells, and batteries) are composed of polycrystalline semiconductor and metal electrodes. The shape and size of the individual crystals constituting a polycrystalline electrode as well as the overall interfacial architecture have a significant effect on the overall performance of the electrode. Therefore, a method that can precisely control electrode morphologies and provide an understanding of their effects on electrode performance is critical for producing highly efficient and cost-effective electrode materials. Electrochemical synthesis is a low-cost method that can produce a variety of materials as polycrystalline electrodes with exceptional control of their morphologies. This article reviews recently developed electrochemical synthesis strategies that produce inorganic materials with various morphological features, which have a direct impact on the material's properties. This article will serve as a good foundation for those seeking a viable electrochemical route to produce electrodes having a specifically desired morphology.