We systematically investigate the effects of Au substrates on the oxygen evolution activities of cathodically electrodeposited nickel oxyhydroxide (NiOOH), nickel–iron oxyhydroxide (NiFeOOH), and nickel–cerium oxyhydroxide (NiCeOOH) at varying loadings from 0 to 2000 nmol of metal/cm2. We determine that the geometric current densities, especially at higher loadings, were greatly enhanced on Au substrates: NiCeOOH/Au reached 10 mA/cm2 at 259 mV overpotential, and NiFeOOH/Au achieved 140 mA/cm2 at 300 mV overpotential, which were much greater than those of the analogous catalysts on graphitic carbon (GC) substrates. By performing a loading quantification using both inductively coupled plasma optical emission spectrometry and integration of the Ni2+/3+ redox peak, we show that the enhanced activity is predominantly caused by the stronger physical adhesion of catalysts on Au. Further characterizations using impedance spectroscopy and in situ X-ray absorption spectroscopy revealed that the catalysts on Au exhibited lower film resistances and higher number of electrochemically active metal sites. We attribute this enhanced activity to a more homogeneous electrodeposition on Au, yielding catalyst films with very high geometric current densities on flat substrates. By investigating the mass and site specific activities as a function of loading, we bridge the practical geometric activity to the fundamental intrinsic activity.