Thin gold films and coatings on metal have long constituted an important technology for the microelectronics industry and will continue to be important for microdevices such as contact springs. The properties of these materials may be highly processing dependent, particularly when the gold is deposited by electrochemical means. In this study, we characterize gold electrodeposited on Ni substrates from two bath chemistries: hard Au sulfite with proprietary hardening additive and soft Au cyanide. TEM and SEM show that the bath chemistry alters the microstructure and the resulting surface of the electrodeposits. Nanoindentation techniques were used to determine the elastic and plastic properties of the Au electrodeposits as a function of the specifics of processing. Soft Au electrodeposits have a grain size of on the order of 300 nm and a hardness of about 1 GPa. Hard Au electrodeposits produced from the sulfite bath feature grain sizes as small as 30 nm, some twinning, and fine porosity uniformly distributed both within the grains and at grain boundaries. The hardness is about 2 GPa, approaching the hardest values reported for sputtered gold films. The effect of the hardening agent on the microstructure of electrodeposits from the Au sulfite bath was also investigated and found to significantly refine the grain size at concentrations of at least 4 mL/L, although little additional refinement was found at higher concentrations.