Hydrogenated microcrystalline (µc) Si/Ge heterostructures were prepared on quartz substrates by plasma-enhanced chemical vapor deposition (CVD) from VHF inductively coupled plasma of SiH4 just after GeH4 employing Ni nanodots (NDs) as seeds for crystalline nucleation. The crystallinity of the films and the progress of grain growth were characterized by Raman scattering spectroscopy and atomic force microscopy (AFM), respectively. When the Ge films were grown on Ni-NDs at 250 °C, the growth of µc-Ge films with crystallinity as high as 80% was realized without an amorphous phase near the Ge film/quartz substrate interface. After the subsequent Si film deposition at 250 °C, fine grains were formed in the early stages of film growth on µc-Ge films with compositional mixing (µc-Si0.85Ge0.15:H) caused by the release of large lattice mismatch between c-Si and c-Ge. With further increase in Si:H film thickness, the formation of large grain structures accompanied by fine grains was promoted. These results suggest that crystalline Si/Ge heterojunctions can be used for efficient carrier collection in solar cell application.