We formed large grain-size polycrystalline silicon (Si) on various substrates at low temperatures of approximately 400 degreesC by utilizing chemical transport of silicon-hydride species generated by the reaction between a solid Si target and hydrogen (H) atoms. H atoms are generated by the catalytic cracking reaction between H-2 and heated tungsten. We named the method 'catalytic chemical sputtering' from an analogy to the conventional physical sputtering. The Si films deposited on Si, thermal oxide and quartz substrates are polycrystalline, and there is no amorphous phase detected by Raman spectroscopy. The grain size exceeds 1 mum for films on thermal oxide substrates, with a thickness of approximately 1 mum at a substrate temperature of 400 degreesC. These grain sizes are larger than those deposited by other deposition methods at comparable low temperatures.