The organosilicon nanoclusters (OSI) and organogermanium nanocluster (OGE) which have a few nanometer sized silicon or germanium cluster and organic groups bonded to the nanocluster surfaces show solubility in common organic solvents and good film processability by solution coating method. Using the coating films as precursors, inorganic silicon and germanium films were prepared by heat treatment in vacuo and laser annealing. The structural changes of the Si and Ge skeletons of the OSI and OGE by heat treatment and laser annealing were investigated by Raman spectroscopy. The laser-annealed films showed Raman bands assigned to the polycrystalline structure. The micropatterning of polycrystalline Ge by laser direct writing method was demonstrated. The organosoluble OGE is expected to be applicable as a germanium ink which gives polycrystalline Ge film.