Background: In brain tumor surgery, maximal tumor resection is typically desired. This is complicated by infiltrative tumor cells which cannot be visually distinguished from healthy brain tissue. Optical methods are an emerging field that can potentially revolutionize brain tumor surgery through intraoperative differentiation between healthy and tumor tissues. Methods: This study aimed to systematically explore and summarize the existing literature on the use of Raman Spectroscopy (RS), Hyperspectral Imaging (HSI), Optical Coherence Tomography (OCT), and Diffuse Reflectance Spectroscopy (DRS) for brain tumor detection. MEDLINE, Embase, and Web of Science were searched for studies evaluating the accuracy of these systems for brain tumor detection. Outcome measures included accuracy, sensitivity, and specificity. Results: In total, 44 studies were included, covering a range of tumor types and technologies. Accuracy metrics in the studies ranged between 54 and 100% for RS, 69 and 99% for HSI, 82 and 99% for OCT, and 42 and 100% for DRS. Conclusions: This review provides insightful evidence on the use of optical methods in distinguishing tumor from healthy brain tissue.