Purpose: To develop a dynamic contrast-enhanced (DCE) MRI method capable of high spatiotemporal resolution, 3D carotid coverage, and T1-based quantification of contrast agent concentration for the assessment of carotid atherosclerosis using a newly developed Multitasking technique. Methods: 5D imaging with 3 spatial dimensions, 1 T1 recovery dimension, and 1 DCE time dimension was performed using MR Multitasking based on low-rank tensor modeling, which allows direct T1 quantification with high spatiotemporal resolution (0.7 mm isotropic and 595 ms, respectively). Saturation recovery preparations followed by 3D segmented fast low angle shot readouts were implemented with Gaussian-density random 3D Cartesian sampling. A bulk motion removal scheme was developed to improve image quality. The proposed protocol was tested in phantom and human studies. In vivo scans were performed on 14 healthy subjects and 7 patients with carotid atherosclerosis. Kinetic parameters including area under the concentration versus time curve (AUC), v(p), K-trans, and v(e) were evaluated for each case. Results: Phantom experiments showed that T1 measurements using the proposed protocol were in good agreement with reference value (R-2 = 0.96). In vivo studies demonstrated that AUC, v(p), and K-trans in the patient group were significantly higher than in the control group (0.63 +/- 0.13 versus 0.42 +/- 0.12, P < 0.001; 0.14 +/- 0.05 versus 0.11 +/- 0.03, P = 0.034; and 0.13 +/- 0.04 versus 0.08 +/- 0.02, P < 0.001, respectively). Results from repeated subjects showed good interscan reproducibility (intraclass correlation coefficient: v(p), 0.83; K-trans, 0.87; v(e), 0.92; AUC, 0.94). Conclusion: Multitasking DCE is a promising approach for quantitatively assessing the vascularity properties of the carotid vessel wall.