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Lipoprotein-associated phospholipase A₂ (Lp-PLA₂), specifically Group VIIA PLA₂, is a member of the phospholipase A₂ superfamily and is found mainly associated with LDL and HDL in human plasma. Lp-PLA₂ is considered as a risk factor, a potential biomarker, a target for therapy in the treatment of cardiovascular disease, and evidence suggests that the level of Lp-PLA₂ in plasma is associated with the risk of future cardiovascular and stroke events. The differential location of the enzyme in LDL/HDL lipoproteins has been suggested to affect Lp-PLA₂ function and/or its physiological role and an abnormal distribution of the enzyme may correlate with diseases. Although a mutagenesis study suggested that a surface helix (residues 362–369) mediates the association between Lp-PLA₂ and HDL, the molecular details and mechanism of association has remained unknown. We have now employed hydrogen …