AbstractDevelopment of devices and structures based on the layered 2D materials critically hinges on the capability to induce, control and tailor the electronic, transport and optoelectronic properties via defect engineering, much like doping strategies have enabled semiconductor electronics and forging enabled introduction the of iron age. Here, we demonstrate the use of a scanning helium ion microscope (HIM) for tailoring the functionality of single layer MoSe₂ locally and decipher associated mechanisms at the atomic level. We demonstrate He⁺ beam bombardment that locally creates vacancies, shifts the Fermi energy landscape and increases the Young’s modulus of elasticity. Furthermore, we observe for the first time, an increase in the B-exciton photoluminescence signal from the nanoforged regions at the room temperature. The approach for precise defect engineering demonstrated here opens opportunities for creating functional 2D optoelectronic devices with a wide range of customizable properties that include operating in the visible region.