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Lipoprotein, especially high-density lipoprotein (HDL), particles are composed of multiple heterogeneous subgroups containing various proteins and lipids. The molecular distribution among these subgroups is closely related to cardiovascular disease (CVD). Here, we established high-resolution proteomics and lipidomics (HiPL) methods to depict the molecular profiles across lipoprotein (Lipo-HiPL) and HDL (HDL-HiPL) subgroups by optimizing the resolution of anion-exchange chromatography (AEC) and comprehensive quantification of proteins and lipids on omics level. Furthermore, based on the Pearson correlation coefficient (PCC) analysis of molecular profiles across high-resolution subgroups, we achieved the relationship of proteome‒lipidome connectivity (PLC) for lipoprotein and HDL particles. By application of these methods to high fat high cholesterol (HFHC) diet-fed rabbits and acute coronary syndrome (ACS) patients, we uncovered the delicate dynamics of molecular profile and reconstruction of lipoprotein and HDL particles. Of note, the PLC features revealed by HDL-HiPL method discriminated ACS from healthy individuals better than direct proteome and lipidome quantification or PLC features revealed by Lipo-HiPL method, suggesting their potential in ACS diagnosis. Together, we established HiPL methods to trace the dynamics of molecular profile and PLC of lipoprotein and even HDL during the development of CVD.

HDL quality features revealed by proteome‒lipidome connectivity are associated with atherosclerotic disease