This article reviews the methodological aspects of detecting low-abundant J-coupled metabolites via 1D spectral editing techniques and 2D nuclear magnetic resonance (NMR) methods applied in vivo, in humans, with a focus on the brain. A brief explanation of the basics of J-evolution will be followed by an introduction to 1D spectral editing techniques (e.g., J-difference editing, multiple quantum coherence filtering) and 2D-NMR methods (e.g., correlation spectroscopy, J-resolved spectroscopy). Established and recently developed methods will be discussed and the most commonly edited J-coupled metabolites (e.g., neurotransmitters, antioxidants, onco-markers, and markers for metabolic processes) will be briefly summarized along with their most important applications in neuroscience and clinical diagnosis.