Iodine is one of the key elements that must be removed from the off-gas systems of nuclear fuel reprocessing. This study systematically investigates the iodine vapor adsorption performance of the metal-organic framework (MOF) material HKUST-1(1-(2-methyl-4-(2-oxopyrrolidin-1-yl)phenyl)-3-morpholino-5,6-dihydropyridin-2(1H)-one), with particle sizes of 100 nm and 20 μm. HKUST-1 samples with varying particle sizes were synthesized via a hydrothermal method. The experimental results show that the 20 μm HKUST-1 exhibits superior crystallinity, a more intact pore structure, and a higher iodine adsorption capacity, reaching 700 mg/g, which is significantly greater than the 300 mg/g capacity of the 100 nm HKUST-1. Kinetic analysis reveals that the adsorption process follows the pseudo-second-order model, with physical adsorption as the predominant mechanism, where iodine molecules are accommodated within the pores. FTIR and XRD further confirm the structural stability of the HKUST-1 framework after iodine adsorption. However, desorption experiments show that iodine molecules are easily volatilized into the air, with a 20% weight loss observed within 10 h and a color change from black to green. The results provide experimental evidence for optimizing the application of HKUST-1 materials in iodine capture and suggest that material modification could enhance the long-term stability of iodine fixation.