Brain phospholipids can be quantitated by high‐resolution 31P NMR of crude brain tissue extracts in the solvent system chloroform‐methanol‐water (+EDTA) which was introduced recently (P. Meneses and T. Glonek, J. Lipid Res. 29, 679 (1988)). Phospholipid resonance positions depend on the type of tissue extract and on solvent composition. The effects of systematic variation of the solvent system on phospholipid NMR profiles are presented. Resolution can be optimized by adjustment of the solvent composition. Virtually all phospholipid classes can be resolved, and the major phospholipids in brain: sphingo‐myelin and phosphatidyl‐choline, ‐serine, ‐inositol, ‐ethanolamine, and ‐ethanolamine plasmalogen can be quantitated easily. Additional resonances have been assigned to phosphatidylcholine plasmalogen, alkylacyl‐phosphatidylcholine and phosphatidylinositolbis‐phosphate. NMR offers a rapid method for quantitative analysis of the phospholipid composition in brain tissue which requires minimum sample handling.