Therefore, the present research study was proposed based on the rationale that many fat-soluble nutrients (carotenoids, vitamins A, E, K, and fatty acids [FA]) are present in human brain (26–31), and that they are a part of dietary patterns and serum NPs previously reported to be associated with better cognitive function in multiple aging cohorts (2, 15, 26, 28, 32, 33). This was accomplished by constructing a posteriori NPs of fat-soluble nutrients measured in brain tissues acquired post-mortem from a subset of centenarians (defined as ≥98 years) who were enrolled in the Georgia Centenarian Study (GCS)—the longest running centenarian study in the U.S. to date (34, 35). Subsequently, the relationship between constructed NPs and cognitive performance at the time point closest to death was cross-sectionally investigated. Findings from this novel study may also provide insights into the role of nutrition in cognition in the oldest old, which may be similar or different from lesser aged older adults.