The present chapter is devoted to the study of amorphous (a-Si:H), polymorphous (pmSi:H), and microcrystalline (μc-Si:H) silicon, deposited by the plasma-enhanced chemical vapor deposition (PECVD) technique at low temperatures. We have studied the main deposition parameters that have strong influence on the optical, electrical, and structural properties of the polymorphous and microcrystalline materials. Our results reveal the key deposition conditions for obtained films with optical and electrical characteristics, which are suitable for applications on thin-film solar cells and semiconductor devices.