We have successfully used hydrophobic direct wafer bonding along with hydrogen-induced layer splitting of germanium to transfer 700 nm thick, single-crystal germanium (100) films to silicon (100) substrates without using a metallic bonding layer. The metal-free nature of the bond makes the bonded wafers suitable for subsequent epitaxial growth of layered solar cells at high temperatures without concern about metal contamination of the device active region. Contact mode atomic force microscopy images of the transferred germanium surface generated by the formation of micro-bubbles and micro-cracks along the hydrogen-induced layer-splitting interface reveals minimum rms surface roughness of between 10 nm and 23 nm. Electrical measurements indicated ohmic I-V characteristics for germanium layers bonded to silicon substrates with ∼400 Ω cm−2 resistance at the interface. Triple-junction solar cell structures grown on these Ge/Si heterostructure templates by metal-organic chemical vapor deposition show comparable photoluminescence intensity and minority carrier lifetime to a control structure grown on bulk Ge. The use of a molecular beam epitaxy Ge buffer layer to smooth the cleaved surface of the Ge heterostructure has been shown to smooth the rms surface roughness from ∼11 nm to as low as 1.5 nm with a mesa-like morphology that has a top surface roughness of under 1.0 nm giving a promising surface for improved solar cell growth on solar cell structures.