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It is hypothesized that plasma proportion of selected fatty acids (FAs) and dietary habits are linked with the risk of cardiovascular disease (CVD) in postmenopausal women. Therefore, this study was designed to determine the association of plasma FA composition and markers of dietary habits with an atherogenic index of plasma (AIP), a predictor of CVD risk in postmenopausal women. In total, 87 postmenopausal women with an average age of 57 ± 7 years were recruited and their dietary intake, anthropometric and biochemical parameters, and FA status in total plasma lipid proportions were determined, showing that 65.5% of the participants had a high risk of CVD according to their AIP value. After adjusting for some confounders (age, body mass index, and physical activity level), the risk of CVD was only positively associated with the frequency of consumption of animal fat spreads (butter and lard) of terrestrial origin. Regarding the FA profile, CVD risk was positively associated with the percentages of vaccenic acid, dihomo-γ-linolenic acid, and monounsaturated fatty acids (MUFA; mainly n-7) in total FA, as well as the MUFA/SFA ratio in total plasma and stearoyl-CoA desaturase-16 activity (16:1/16:0 ratio). In contrast, the risk of CVD was negatively associated with percentages of α-linolenic acid, total polyunsaturated fatty acids (PUFA), and PUFA/MUFA ratio in total plasma lipid, and the estimated activity of Δ5-desaturase (20:4/20:3 n-6 ratio). These results support the current recommendations to decrease the frequency of animal fat spread intake because it is associated with a reduced CVD risk based on AIP in postmenopausal women. In accordance with these plasma percentages of ALA, vaccenic acid, dihomo-γ-linolenic acid, PUFA, PUFA/MUFA ratio, and 16:1/16:0 ratio may be important parameters in CVD risk assessment.