This chapter addresses fundamental technological considerations followed by a discussion of what molecular and metabolic information can be obtained from 31P and 1H magnetic resonance spectroscopy (MRS). This is followed by a selective review of the literature to date on 31P and 1H MRS studies in schizophrenia. In a proton-coupled in-vivo 31P brain spectrum, the resonances that are reliably quantifiable include phosphomonoester (PME), inorganic orthophosphate (Pi), phosphodiester (PDE), phosphocreatine (PCr), γ-adenosine-50-triphosphate (γATP), αATP, and βATP. The PME and PDE levels from the short nuclear magnetic resonance (NMR) correlation time components provide a measure of membrane phospholipid metabolism. The in-vivo 1H MRS spectrum contains three major resonance regions. Many neurochemical, neuropathological and functional imaging studies have implicated the frontotemporal neural networks in schizophrenia. Most of the in-vivo 1H MRS findings in schizophrenia focus on changes in N-acetyl aspartate (NAA), the largest resonance in 1H MRS spectra.