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Background Obtaining ventricular volumetry and mass is key to most cardiac MRI but challenged by long multibreath-hold acquisitions. Purpose To assess the image quality and performance of a highly accelerated, free-breathing, two-dimensional cine cardiac MRI sequence incorporating deep learning (DL) reconstruction compared with reference standard balanced steady-state free precession (bSSFP). Materials and Methods A DL algorithm was developed to reconstruct custom 12-fold accelerated bSSFP cardiac MRI cine images from coil sensitivity maps using 15 iterations of separable three-dimensional convolutions and data consistency steps. The model was trained, validated, and internally tested in 10, two, and 10 adult human volunteers, respectively, based on vendor partner-supplied fully sampled bSSFP acquisitions. For prospective external clinical validation, consecutive children and young adults undergoing cardiac MRI from September through December 2019 at a single children's hospital underwent both conventional and highly accelerated short-axis bSSFP cine acquisitions in one MRI examination. Two radiologists scored overall and volumetric three-dimensional mesh image quality of all short-axis stacks on a five-point Likert scale and manually segmented endocardial and epicardial contours. Scan times and image quality were compared using the Wilcoxon rank sum test. Measurement agreement was assessed with intraclass correlation coefficient and Bland-Altman analysis. Results Fifty participants (mean age, 16 years ± 4 [standard deviation]; range, 5-30 years; 29 men) were evaluated. The mean prescribed acquisition times of accelerated scans (non-breath-held) and bSSFP (excluding breath-hold time) were 0.9 minute ± 0.3 versus 3.0 minutes ± 1.9 (<i>P</i> < .001). Overall and three-dimensional mesh image quality scores were, respectively, 3.8 ± 0.6 versus 4.3 ± 0.6 (<i>P</i> < .001) and 4.0 ± 1.0 versus 4.4 ± 0.8 (<i>P</i> < .001). Raters had strong agreement between all bSSFP and DL measurements, with intraclass correlation coefficients of 0.76 to 0.97, near-zero mean differences, and narrow limits of agreement. Conclusion With slightly lower image quality yet much faster speed, deep learning reconstruction may allow substantially shorter acquisition times of cardiac MRI compared with conventional balanced steady-state free precession MRI performed for ventricular volumetry. © RSNA, 2021 <i>Online supplemental material is available for this article.</i>