Molecular imaging of brain metastases with positron emission tomography with computed tomography (PET/CT) or with magnetic resonance imaging (PET/MRI) can be performed with a growing number of molecular imaging agents. The most commonly used molecular imaging agent for primary malignancies outside of the brain is a glucose analog radio-labelled with fluorine-18, 18F-fluorodeoxyglucose (18F-FDG), which can be used to identify brain metastases. Likewise, additional molecular imaging agents such as prostate specific membrane antigen (PSMA) ligands (i.e., 68Ga-PSMA-11), alkylphosphocholine analogs (i.e., CLR124/CLR1404), and amino acids (i.e., 11C-MET, 18F-FET, 18F-DOPA, 18F-FACBC) can identify brain metastases. Advantages of PET in brain tumor imaging include co-registration with other imaging technologies, quantitative measurements, and significant potential for improvement in diagnostic accuracy. PET can be used to detect brain metastases while imaging for other Note to the Reader: This chapter is part of the book Metastasis (ISBN: 978-0-6453320-2-5), scheduled for publication in April 2022. The book is being published by Exon Publications,