The silicon-substituted polysilane(SPS) as a novel class of polysilane was prepared by (polymer) reaction of polymethylsilane(PMS) with substitution degree being 43% and characterized by FT-IR, ~(1)H NMR, ~( 29)Si CP MAS-NMR, UV and GPC techniques. The polymer is soluble in common organic solvents, and its molecular weight could be increased by crosslinking reaction.