Metal-organic framework (MOF) glass is a new type of glass material, but it usually lacks sufficient porosity. Thus, regulating the pore structure of MOF glass to improve its adsorption performance is very important. Herein, we found that the porosity of MOF glasses agZIF-62 and agZIF-76 can be regulated via an ammonia-immersion approach. After ammonia immersion, the resulting agZIF-62-NH3 and agZIF-76-NH3 could be maintained in their glass states or converted to their amorphous states, respectively. Their porosity changed according to the gas adsorption experiments. Notably, compared with agZIF-62 and agZIF-76, the iodine uptake capacities for agZIF-62-NH3 and agZIF-76NH3 increased by 12 and 21 times, respectively. This work shows that the subsequent treatment of MOF glass can regulate their adsorption performance.