Chemical compositions, unit-cell contents, and optical properties of six clinopyroxenes from the Upper Layered Series are presented. There is a gradual enrichment in iron upwards in the intrusion although there is no measurable effect on the optical properties, possibly because of Cr variation and exsolution of Fe and Ti as oxides. The chemistry of the clinopyroxenes is consistent with crystallization from a water-rich magma of transitional nature between tholeiite and alkali-olivine basalt. X-ray oscillation photographs of single crystals reveal the presence of sub-microscopic exsolution lamellae of pigeonite, a feature consistent with the transitional nature of the parent magma. Exsolution lamellae of titanomagnetite are ubiquitous and were formed at subsolidus temperatures in response to high buffered oxygen fugacity. Comparisons are made between the properties of clinopyroxenes from the Lower, Middle, and Upper Layered Series, and the conditions of crystallization of each series.