The border zone of post-infarction myocardial scar as identified by late gadolinium enhancement (LGE) has been identified as a substrate for arrhythmias and consequently, high-resolution 3D scar information is potentially useful for planning of electrophysiological interventions. This study evaluates the performance of a novel high-resolution 3D self-navigated free-breathing inversion recovery magnetic resonance pulse sequence (3D-SN-LGE) vs. conventional 2D breath-hold LGE (2D-LGE) with regard to sharpness of borders (SBorder) of post-infarction scar. Patients with post-infarction scar underwent two magnetic resonance examinations for conventional 2D-LGE and high-resolution 3D-SN-LGE acquisitions (both 15 min after 0.2 mmol/kg Gadobutrol IV) at 1.5T. In the prototype 3D-SN-LGE sequence, each ECG-triggered radial steady-state-free-precession read-out segment is preceded by a non-slice-selective inversion pulse. Scar volume and SBorder were assessed on 2D-LGE and matching reconstructed high-resolution 3D-SN-LGE short-axis slices. In 16 patients (four females, 58 ± 10y) all scars visualized by 2D-LGE could be identified on 3D-SN-LGE (time between 2D-LGE and 3D-SN-LGE 48 ± 53 days). A good agreement of scar volume by 3D-SN-LGE vs. 2D-LGE was found (Bland-Altman: -3.7 ± 3.4 ml, correlation: r = 0.987, p < 0.001) with a small difference in scar volume (20.5 (15.8, 35.2) ml vs. 24.5 (20.0, 41.9)) ml, respectively, p = 0.002] and a good intra- and interobserver variability (1.1 ± 4.1 and -1.1 ± 11.9 ml, respectively). SBorder of border "scar to non-infarcted myocardium" was superior on 3D-SN-LGE vs. 2D-LGE: 0.180 ± 0.044 vs. 0.083 ± 0.038, p < 0.001. Detection and quantification of myocardial scar by 3D-SN-LGE is feasible and accurate in comparison to 2D-LGE. The high spatial resolution of the 3D sequence improves delineation of scar borders.