A 75-year-old woman with papillary thyroid carcinoma who underwent 131I radioiodine treatment was incidentally found to have an established left cerebral infarct demonstrating 131I uptake on posttherapy whole-body scan. False-positive iodine accumulation can occur in benign processes and other malignancies, necessitating awareness among nuclear medicine physicians to avoid misdiagnosing metastatic disease. SPECT/CT can be utilized to enhance diagnostic accuracy when needed.