The growth of uniform gallium nitride (GaN) thin films was reported on (100) Si substrate by remote plasma atomic layer deposition (RP-ALD) using triethylgallium (TEG) and NH3 as the precursors. The self-limiting growth of GaN was manifested by the saturation of the deposition rate with the doses of TEG and NH3. The increase in the growth temperature leads to the rise of nitrogen content and improved crystallinity of GaN thin films, from amorphous at a low deposition temperature of 200 °C to polycrystalline hexagonal structures at a high growth temperature of 500 °C. No melting-back etching was observed at the GaN/Si interface. The excellent uniformity and almost atomic flat surface of the GaN thin films also infer the surface control mode of the GaN thin films grown by the RP-ALD technique. The GaN thin films grown by RP-ALD will be further applied in the light-emitting diodes and high electron mobility transistors on (100) Si substrate.