A two‐dimensional (2D) chemical shift correlated MR spectroscopic (COSY) sequence integrated into a new volume localization technique (90°–180°–90°) is proposed for whole‐body MR spectroscopy (MRS). Using the product operator formalism, a theoretical calculation of the volume localization as well as the coherence transfer efficiencies in 2D MRS is presented. Phantom model solutions were used to test and optimize the efficiency of the proposed sequence. A combination of different MRI transmit/receive RF coils was used: a head MRI coil and a 3″ surface coil receive combined with a body coil transmit. The J cross‐peaks due to N‐acetyl aspartate (NAA), glutamate/glutamine (Glx), myo‐inositol (mI), creatine (Cr), choline (Ch), aspartate (Asp), γ‐aminobutyrate (GABA), taurine (Tau), glutathione (GSH), threonine (Thr), and macromolecules (MM) were identified. The cross‐peak intensities excited by the proposed 2D sequence were asymmetric with respect to the diagonal peaks. Localized COSY (L‐COSY) spectra of cerebral prefrontal and occipital gray/white matter regions in 15 healthy controls are presented. Magn Reson Med 46:58–67, 2001. © 2001 Wiley‐Liss, Inc.