(Figure Presented) To date, the chemical vapor deposition (CVD) process is the most popular approach because of its high yield and quality. Nevertheless, the need for a high temperature and the relatively long process time within each cycle hinder the commercial development in terms of production cost. In this work, we demonstrate a fast (<3 min) and feasible approach to synthesizing a few-layers of WSe2 and MoSe2 on arbitrary substrates by a microwave-assisted selenization process. The transition metal dichalcogenides (TMDs) can be patterned by standard photolithography. Furthermore, controllable layered growth from horizontal to vertical alignment can be achieved, leading to an enhanced chemical catalytic activity caused by large edge sites (exposed areas). As a proof, a highly sensitive NO gas sensor based on vertical WSe2 was fabricated. Moreover, our microwave-assisted selenization process can be further extended to achieve other two-dimensional TMD materials because of the simplicity of the process.