Because of the increasing use of the neopentyl polyol esters as lubricants, an analytical method capable of giving detailed information concerning the composition of these complex ester mixtures is desirable. Methods of gas-liquid chromatography and thin-layer chromatography have been applied in the successful development if such an analytical method. By direct programmed temperature gas chromatography of the lubricants, the components are separated according to volatility; in most cases resolution is adequate for semi-quantitative analysis. Gas-liquid chromatographic analysis of the free acids produced by hydrolysis of the sample reveals the acyl composition. The parent polyols are determined by programmed temperature gas chromatography of their valerate esters. A semi-preparative thin-layer chromatographic method permits the isolation of the three main ester types, trimethylol propane, pentaerythritol, and dipentaerythritol, for further analysis. A combination of these analytical methods permits a detailed study of the changes in composition which occur in these lubricants during service.Presented at the 24th ASLE Annual Meeting in Philadelphia, May 5–9, 1969.