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Gliomas are infiltrative lesions that typically have poorly defined margins on conventional magnetic resonance (MR) and computed tomography (CT) images. This presents a considerable challenge for planning radiation and other forms of focal therapy, and introduces the possibility of both under‐treating macroscopic tumor, and over‐treating regions of normal brain tissue. New therapy systems are able to deliver radiation more precisely and accurately to irregular three‐dimensional target volumes, and have placed a premium on definition of the spatial extent of the lesion. Proton MR spectroscopic imaging (H‐MRSI) has been proposed as an in vivo molecular imaging technique that assists in targeting and predicts response to radiation therapy for patients with gliomas. The evidence that supports the use of H‐MRSI for planning radiation treatment is reviewed, together with the technical requirements for …