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This study aimed to prospectively evaluate delayed enhancement imaging by spectral computed tomography using soluble iodine containing contrast media to improve the in vivo characterization of coronary plaque types based on the quantification of delayed iodine enhancement. Patients with known or suspected coronary artery disease (CAD) underwent spectral coronary CT-angiography (SCCTA). Absolute delayed iodine enhancement in all visible coronary plaques was assessed. Patients with significant CAD (> 50% stenosis) further underwent invasive coronary angiography (ICA) including optical coherence tomography (OCT). We identified 50 non-calcified coronary plaques in 72 patients undergoing SCCTA. 17 patients with significant CAD underwent further ICA including OCT imaging. In those, we were able to match 35 plaques by both SCCTA and OCT. Based on OCT imaging, 22/35 matched plaques (63%) were characterized as high-risk coronary plaques (thin-cap fibroatheroma n = 2, fibroatheroma n = 20), whereas 13/35 (37%) were characterized as low-risk plaques (fibrocalcific lesion n = 3, fibrous plaques n = 9, and early-onset fibroatheroma n = 1). All plaques showed similar HU’s and could not be classified into high-risk or low-risk plaques by conventional CT measures. Minimal delayed iodine enhancement within plaques as quantified by SCCTA demonstrated significantly lower values in high-risk as compared to low-risk coronary plaques (1.0 ± 1.5 mg/ml vs. 2.2 ± 1.1 mg/ml, p = 0.021) which allowed estimation of high-risk plaques with high sensitivity and moderate specificity (77% and 56%). Measurement of delayed enhancement iodine uptake within stable coronary artery plaques using dual-layer SCCTA might contribute to a more precise estimation of plaque vulnerability surpassing conventional CT techniques.