The aim of this study was to introduce a novel method combining contrast-enhanced magnetic resonance angiography (CE-MRA), short inversion time inversion recovery sampling perfection with application-optimized contrasts using different flip angle evolutions (T2-STIR-SPACE) and volumetric interpolated breath-hold examination (VIBE) sequences in the assessment of thoracic outlet syndrome (TOS). Material/Methods: CE-MRA, T2-STIR-SPACE, and VIBE techniques were employed to evaluate neurovascular bundles in 27 patients clinically suspected of TOS. Images were evaluated to determine the cause of neurovascular bundle compression. Surgical exploration was performed in patients with abnormal magnetic resonance imaging (MRI) results. Results: Twenty patients were found to be abnormal: 6 cases showed only neurogenic TOS and the correlates included infraclavicular hemangiomas (n=1) and transverse cervical artery (n=5). Arterial-neurogenic TOS was found in 4 cases, including subclavian lymph node metastasis from breast cancer (n=3) and schwannoma (n=1). Arterial-venous-neurogenic TOS was found in 1 subject, and the correlates included a fibrous band from the cervical rib and elongated C7 transverse process. In this case, the subclavian artery/vein was compressed dynamically. Venous-neurogenic TOS was noted in one subject. Nine patients were considered as post-traumatic TOS, including brachial plexus edema (n=3), the brachial plexus rupture (n=2), peri-brachial plexus effusion (n=3), and stenosis of the SCA (n=1). In the remaining 7 patients, MRI did not detect abnormalities. Conclusions: TOS can be evaluated by CE-MRA, T2-STIR-SPACE, and VIBE during a single examination, with a reduced contrast material dose. This imaging modality performs well in showing the anatomical structure of the neurovascular bundle and the cause of the compression.