Background: Thallium-201 single-photon emission computed tomography/computed tomography(SPECT/CT) brain scan is an imaging modality which can be done to differentiate between malignant and nonmalignant lesions among patients with nonconclusive findings on conventional neuroimaging. This study describes the results of thallium-201 SPECT/CT brain imaging and relate it to histopathologic and/or clinical findings and evaluate the value of thallium-201 SPECT/CT brain imaging in differentiating malignant from nonmalignant lesions. Methods: This is a retrospective case series study of 10 patients with cerebral lesions who un-derwent thallium-201 SPECT/CT brain imaging in a hospital in the Philippines from 2010 to 2021. Results: A total of 10 patients underwent thallium-201 SPECT/CT brain scan. Six had nega-tive results while 4 had positive results. All of the patients who had positive results were found to have malignancy, whether recurrent or newly diagnosed. All of the patients with negative scan were found to have either an infectious and inflammatory disease and responded to treatment albeit in different degrees. Two of the 10 patients underwent biopsy whose results were consistent with the thallium-201 SPECT/CT brain scan results. Conclusion Thallium-201 brain scan combined with SPECT and SPECT/CT has been demon-strated to be useful in distinguishing malignant from nonmalignant lesions and is more cost-effective versus other imaging techniques. The findings in this study support the role of thallium scintigraphy in the diagnosis of patients with brain lesions most significantly when there is a need to differentiate between a malignant and benign condition.