In various methods to determine alpha-emitting radionuclides in matrices, alpha-particle spectrometry with alpha-emitting sources prepared by the electrodeposition has been widely used. Although there are several good review papers on alphaparticle spectrometry and preparation of electrodeposited alpha-emitting sources, the mechanism of analysis procedure and characterizations of alpha-emitting sources have not been reported well. These untouched subjects by other review papers are very significant to improve the analysis procedure. This review focuses on the mechanism of the electrodeposition of alpha-emitting radionuclides on the stainless steel disc, factors for the preparation of electrodeposited alpha-emitting layers, and various characterization methods.