Magnetic resonance spectroscopy (MRS) and spectroscopic imaging (MRSI) are valuable tools to detect metabolic changes in tumors. The currently emerging era of molecular medicine, which is shaped by molecularly targeted anticancer therapies combined with molecular imaging of the effects of such therapies, requires powerful imaging technologies that are able to detect molecular information. MRS and MRSI (MRS/I) are such technologies that are able to detect metabolites arising from glucose and choline metabolism in noninvasive in vivo settings and at higher resolution in tissue samples. The roles that MRS/I plays in diagnosing different types of cancer as well as in early monitoring of tumor response to traditional chemotherapies are reviewed. Emerging roles of MRS/I in the development and detection of novel targeted anticancer therapies that target oncogenic signaling pathways or targets in choline or glucose metabolism are discussed.