Background: To investigate the predictive accuracy of three-dimension (3D) time-of-flight (TOF) MR angiography (MRA) and 3D Fast Imaging Employing Steady-state Acquisition (FIESTA) techniques in assessing neurovascular compression (NVC) with specific vessels in patients with primary trigeminal neuralgia (TN). Methods: Patients with single-site primary TN undergoing microvascular decompression (MVD) were retrospectively recruited. All patients had available preoperative magnetic resonance imaging (MRI) scans. A quantitative NVC scoring system was applied to assess the severity of NVC on MRI. The radiological findings were correlated with the intraoperative result to determine the diagnostic accuracy of MRI techniques. Besides, the radiological indicator of MVD was determined. Results: Seventy-three TN patients were recruited. Thirty-three patient had bilateral NVC but with unilateral neuralgia. The average NVC score of the asymptomatic side was significantly lower than that of the symptomatic side (1.6 vs. 6.7; p 0.001). A cut-off value of NVC >4 was determined as a radiological indicator of MVD with sensitivity and specificity of 82.2% and 98.6%, respectively Area Under Curve (AUC = 0.97; p 0.001). Approximately 90% of symptomatic patients had the distance to REZ \le3 mm. 68.5% of patients had a single conflicting vessel, and superior cerebellar artery (SCA) was the predominate vessel (46.6%). The sensitivity and specificity of MRI to detect NVC were 95.8% and 100%, respectively. Regarding each vessel, the cohen’s kappa statistic (K) was 0.632 overall. Conclusions: 3D TOF MRA and FIESTA show an overall good ability to predict specific offending vessels. NVC score >4 is identified to predict TN, suggestive of subsequent surgical treatment.