The aim of this study was to investigate the possibility of 64-slice multislice computed tomography (MSCT) to detect vulnerable plaque derived by optical coherence tomography. From September 2007 through December 2009, 122 lesions in 81 patients were evaluated by 64-slice MSCT and optical coherence tomography. Based on optical coherence tomographic findings, lesions were classified as thin-capped fibroatheroma (TCFA; n = 37) and non-TCFA (n = 85). Mean computed tomographic density value of the lesion was lower and remodeling index was larger in the TCFA group (44.9 ± 19.2 vs 78.7 ± 25.0 HU, p <0.0001; 1.14 ± 0.20 vs 0.95 ± 0.16, p <0.0001, respectively). Mean computed tomographic density value was correlated and remodeling index was inversely correlated with fibrous cap thickness (r = 0.605, p <0.0001; r = −0.591, p <0.0001, respectively). Optimal threshold of mean computed tomographic value and remodeling index identified by receiver operating characteristic curve were 62.4 HU and 1.08 (area under the curve 0.859 and 0.781). Signet ringlike appearance was observed more frequently in the TCFA group (65% vs 16%, p <0.0001). In multivariate analysis, independent predictors of TCFA were mean computed tomographic density value ≤62.4 HU (odds ratio 8.20, 95% confidential interval 2.49 to 27.0, p = 0.0005), remodeling index ≥1.08 (odds ratio 6.10, 95% confidential interval 2.04 to 18.2, p = 0.0012), and signet ringlike appearance (odds ratio 6.33, 95% confidential interval 2.03 to 19.7, p = 0.0014). In conclusion, based on comparisons with optical coherence tomographic findings, 64-slice MSCT may have the potential to detect vulnerable plaque.