Abstract Metal‐organic frameworks (MOFs) glass is a newly invented hybrid materials with the unique optical response and great potential for photonic applications. Unfortunately, limited by the high viscosity and instability issue of the ZIF‐62 precursor, the controllable synthesis of homogeneous MOFs glass remains a significant challenge. In this manuscript, it is found that reducing the stoichiometric ratio between Zn ions and the ligand precursor can effectively suppress the growth of the ZIF‐62 and enable to obtain tiny precursor particles. By using them, the homogenous MOFs glass free of bubbles can be fabricated by gentle heat‐treatment. This hybrid MOFs glass exhibits interesting optical response, including intense luminescence, atmosphere sensitive optical response and high energy particle scintillating emission. The applications for active atmosphere sensing and neutron detection with extremely high signal‐to‐noise ratio of 27.1 dB are demonstrated. The results suggest that homogenous amorphization of MOFs may create a new type of photonic material with unprecedent optical response and significant sensing application.