This invention provides a process for producing a high-purity sphingomyelin and a high-purity plasmalogen-form glycerophospholipid from a biological material by simple procedures at high yields. The process comprises the steps of: (A) subjecting dried total lipids extracted from a biological material to extraction treatment with a specific mixture solution to separate an insoluble portion composed mainly of sphingomyelin and a soluble portion; (B) subjecting the insoluble portion, obtained in said Step (A), to washing treatment with a specific mixture solution to obtain crude sphingomyelin; (C) subjecting the soluble portion, obtained in said Step (A), to washing treatment with a water-soluble ketone solvent to obtain crude plasmalogen-form glycerophospholipid; (D) causing an enzyme to act on the crude sphingomyelin, obtained in said Step (B), to obtain sphingomyelin having a purity of 90% or more; and (E) causing an enzyme to act on the crude plasmalogen-form glycerophospholipid, obtained in said Step (C), to obtain plasmalogen-form glycerophospholipid having a purity of 40% or more.