Background: Studies relating cardiovascular outcomes to dietary or blood measures of various fatty acids rely on the implicit assumptions that dietary change results in changes in blood fatty acids that, in turn, alter cardiac fatty acids. Although dietary intakes of n-3 (omega-3), n-6 (omega-6), and trans fatty acids are reflected in their concentrations in blood, there are few human data on the relation between blood and cardiac concentrations of fatty acids. Objective: The objective was to explore relations between blood and myocardial n-3, n-6, trans, monosaturated, and saturated fatty acids over a range of community intakes to evaluate whether blood fatty acids are useful surrogate markers of their cardiac counterparts. Design: Patients undergoing on-pump coronary bypass surgery were recruited. Right atrial appendages and blood were collected at surgery for fatty acid analysis. Results: Atrial appendages and matching blood samples were collected from 61 patients. Highly significant correlations were identified between atrial and erythrocyte or plasma n-3 [eg, eicosapentaenoic acid (erythrocytes: r = 0.93, P < 0.0001; plasma: r = 0.87, P < 0.0001)], some n26 [eg, arachidonic acid (erythrocytes: r = 0.45, P = 0.0003; plasma: r = 0.39, P = 0.002)], trans [eg, total trans 18:1 (erythrocytes: r = 0.89, P < 0.0001; plasma: r = 0.74, P < 0.0001)], and monounsaturated [eg, oleic acid (erythrocytes: r = 0.37, P = 0.003)] fatty acids. There were no statistical associations between blood and cardiac saturated fatty acids. Conclusion: Erythrocyte- and plasma phospholipid-derived fatty acids can be used to estimate cardiac fatty acid status in humans.