Investigation of the metabolic status of the brain is problematic due to its inaccessibility. NMR-based metabolomics offers potential diagnostic capabilities via measurement of brain or related biofluid metabolic profiles. In this review we examine the extent to which NMR and MRS have been employed in studies of neurological disorders, the information obtainable, the strengths and limitations of each technology. The potential for wider application of these complementary technologies in metabolomics research is discussed, both in isolation and in combination. The current status of the statistical framework for dealing with these data sets is also examined and suggestions offered for future directions.