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Understanding the distribution and variation in NMR-based inflammatory markers is crucial to the evaluation of their clinical utility in disease prognosis and diagnosis. We applied high-resolution ¹H NMR spectroscopy of blood plasma and serum to measure the acute phase reactive glycoprotein signals (GlycA and GlycB) and the subregions of the lipoprotein-based Supramolecular Phospholipid Composite signals (SPC₁, SPC₂, and SPC₃) in a large multicohort population study. A total of 5702 samples were studied to determine the signal variations in a range of chronic and acute inflammatory conditions. We found that while GlycA and GlycB were increased in inflammation, the SPC regions behaved independently of Glyc signals, with SPC₂ and SPC₃ being reduced in chronic inflammation in comparison to healthy controls (p-value SPC₂ = 2.9 × 10^-10, p-value SPC₃ = 2.2 × 10^-3) and SPC₁ (p-value = 0.29) being unchanged. SPC₁ was decreased in acute inflammation, indicating a link to the immune response (p-value = 2.5 × 10^-11). These findings confirm the independent biological relevance of all three SPC subregions and contraindicate the use of aggregate SPC values as general inflammatory markers.