We report a new low‐temperature (<300 °C) process for selective deposition of silicon using time modulated flow of silane into a hydrogen plasma. Time modulated gas flow allows the chemical processes associated with deposition and surface modification or etching to occur sequentially, and be controlled independently, giving an additional degree of freedom to the deposition process. The observed selective deposition is consistent with substrate specific nucleation, and preferential etching of the nuclei during the hydrogen plasma exposure. The application of the selective deposition process to the fabrication of thin‐film transistor structures is also presented.