Despite growing interest in doping two-dimensional (2D) transition metal dichalcogenides (TMDs) for future layered semiconductor devices, controllability is currently limited to only heavy doping (degenerate regime). This causes 2D materials to act as metallic layers, and an ion implantation technique with precise doping controllability is not available for these materials (e.g., MoS2, MoSe2, WS2, WSe2, graphene). Since adjustment of the electrical and optical properties of 2D materials is possible within a light (nondegenerate) doping regime, a wide-range doping capability including nondegenerate and degenerate regimes is a critical aspect of the design and fabrication of 2D TMD-based electronic and optoelectronic devices. Here, we demonstrate a wide-range controllable n-doping method on a 2D TMD material (exfoliated trilayer and bulk MoS2) with the assistance of a phosphorus silicate glass (PSG) insulating layer, which has the broadest doping range among the results reported to date (between 3.6 × 1010 and 8.3 × 1012 cm ‑2) and is also applicable to other 2D semiconductors. This is achieved through (1) a three-step process consisting of, first, dopant out-diffusion between 700 and 900 °C, second, thermal activation at 500 °C, and, third, optical activation above 5 μW steps and (2) weight percentage adjustment of P atoms in PSG (2 and 5 wt %). We anticipate our widely controllable n-doping method to be a starting point for the successful integration of future layered semiconductor devices.