We investigate picosecond spin currents across Au/iron-garnet interfaces in response to ultrafast laser heating of the electrons in the Au film. In the picoseconds after optical heating, interfacial spin currents occur due to an interfacial temperature difference between electrons in the metal and magnons in the insulator. We report measurements of this interfacial longitudinal spin Seebeck effect between Au and rare-earth iron-garnet insulators, i.e., RE 3 Fe 5 O 12 , where RE is Y, Eu, Tb, Tm. By systematically varying the rare-earth element, we modify the total magnetic moment of the iron garnet. We use time-domain thermoreflectance measurements to characterize the thermal response of the bilayer to ultrafast optical heating. We use time-resolved magneto-optic Kerr effect measurements of the Au layer to measure the time evolution of spin accumulation in the Au film. Replacing Y with other rare earths enhances the electron-magnon conductance G e−m at the Au iron-garnet interface by as much as a factor of 3. The electron-magnon conductance does not follow the trend of either the total magnetization of the iron garnet or the magnetic moment of the rare earth.