The effective capture and storage of radiological iodine (I-129) remains a strong concern for safe nuclear waste storage and safe nuclear energy. Silver-containing mordenite (MOR) is a longstanding benchmark for iodine capture; however, the molecular level understanding of this process needed to develop more effective iodine getters has remained elusive. Here we probe the structure and distribution of iodine sorbed by silver-containing MOR using differential pair distribution function analysis. While iodine is distributed between gamma-AgI nanoparticles on the zeolite surface and subnanometer alpha-AgI clusters within the pores for reduced silver MOR, in the case of unreduced silver-exchanged MOR, iodine is exclusively confined to the pores as subnanometer alpha-AgI. Consequently, unreduced silver-containing zeolites may offer a more secure route for radioactive iodine capture, with the potential to more effectively trap the iodine for long-term storage.