Purpose: To evaluate the use of low-dimensional-structure self-learning and thresholding (LOST) compressed sensing acquisition and reconstruction in the assessment of left atrial (LA) and left ventricular (LV) scar by using late gadolinium enhancement (LGE) magnetic resonance (MR) imaging with isotropic spatial resolution. Materials and Methods: The study was approved by the local institutional review board and was compliant with HIPAA. All subjects provided written informed consent. Twenty-eight patients (eight women; mean age, 58.0 years ± 10.1) with a history of atrial fibrillation were recruited for the LA LGE study, and 14 patients (five women; mean age, 54.2 years ± 18.6) were recruited for assessment of LV myocardial infarction. With use of a pseudorandom k-space undersampling pattern, threefold accelerated three-dimensional (3D) LGE data were acquired with isotropic spatial resolution and reconstructed off-line by using LOST. For comparison, subjects were also imaged by using standard 3D LGE protocols with nonisotropic spatial resolution. Images were compared qualitatively by three cardiologists with regard to diagnostic value, presence of enhancement, and image quality. The signed rank test and Wilcoxon unpaired two-sample test were used to test the hypothesis that there would be no significant difference in image quality ratings with different resolutions. Results: Interpretable images were obtained in 26 of the 28 patients (93%) in the LA LGE study. LGE was seen in 17 of 30 cases (57%) with nonisotropic resolution and in 18 cases (60%) with isotropic resolution. Diagnostic quality scores of isotropic images were significantly higher than those of nonisotropic images with coronal views (median, 3 vs 2, respectively [25th and 75th percentiles: 3, 3 vs 2, 3]; P < .001) and sagittal views (median, 3 vs 2 [25th and 75th percentiles: 3, 4 vs 2, 3]; P < .001) but lower with axial views (median, 4 vs 3 [25th and 75th percentiles: 3, 4 vs 3, 3]; P < .001). For the LV LGE study, all patients had interpretable images. LGE was seen in six of 14 patients (43%), with 100% agreement between both data sets. Diagnostic quality scores of high-isotropic-resolution LV images were higher than those of nonisotropic images with short-axis views (median, 4 vs 3 [25th and 75th percentiles: 3, 4 vs 2, 3]; P = .014) and two-chamber views (median, 4 vs 3 [25th and 75th percentiles: 3, 4 vs 2, 3]; P = .001). Conclusion: An accelerated LGE acquisition with LOST enables imaging with high isotropic spatial resolution for improved assessment of LV, LA, and pulmonary vein scar.