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SyMRI is a quantitative synthetic MR imaging method where a single saturation recovery TSE sequence is used to estimate the proton density, longitudinal relaxation rate, and transverse relaxation rate and allows for a free range of synthetic weightings. Twenty patients with MS and 20 healthy controls were enrolled and synthetic MR imaging was implemented on a Siemens 3T scanner. Diagnostic accuracy, lesion detection, and artifacts were assessed by blinded neuroradiologic evaluation, and CNR by manual tracing. Synthetic PD-, T1-, and T2-weighted images were of sufficient or good quality and were acquired in 7% less time than with conventional MRI. Synthetic FLAIR images suffered from artifacts. Also, synthetic MRI provided segmentations with the shortest processing time (16 seconds) and the lowest repeatability error for brain volume. Synthetic MRI can be an alternative to conventional MRI for generating diagnostic PD-, T1-, and T2-weighted images in patients with MS with fast and robust volumetric measurements.