To investigate the value of dual-phase head-and-neck computed tomography angiography (CTA) in assessing advantages and risks associated with mechanical thrombectomy for stroke with a large ischemic region in the anterior circulation within 6 h of onset. We retrospectively analyzed the data of patients with acute occlusion of the internal carotid artery or middle cerebral artery-M1 segment. Baseline dual-phase CTA was performed for collateral grading using the 4-point visual collateral score (0, 0% filling; 1, >0% and ≤50% filling; 2, >50 and <100% filling; 3, 100% filling). The rates of modified Rankin score (MRS) ≤ 3 at 90 days, any intracranial hemorrhage (ICH) within 48 h, malignant cerebral edema within 24 h, and all-cause 90-day mortality were analyzed. Among the 69 study patients, 15, 26, 17, and 11 patients had collateral grades of 0, 1, 2, and 3, respectively. At 90 days, the MRS was ≤3 in 0, 8.33, 29.41, and 36.36% of patients with grades 0, 1, 2, and 3, respectively. ICH incidence was 73.33, 57.69, 29.41, and 18.18% for grades 0, 1, 2, and 3, respectively, while the incidence of malignant brain edema was 100, 76.92, 35.29, and 0%, respectively. All-cause 90-day mortality was 53.33% for grade 0 and 30.77% for grade 1; no deaths occurred at grades 2 and 3. Collateral grading based on dual-phase CTA enables simple and rapid preoperative evaluation prior to mechanical thrombectomy for acute anterior-circulation stroke with a large ischemic focus, particularly for patients presenting within the 6-h time window.