Objectives: This study aimed to compare radiotherapy plan quality of coplanar VMAT (CO-VMAT) and non-coplanar VMAT (NC-VMAT) for postoperative primary brain tumour. Methods: A total of 16 patients who were treated for primary brain tumours were retrospectively selected for this study. For each patient, identical CT sets with structures were used for both CO-VMAT and NC-VMAT planning. For CO-VMAT, one full arc and two coplanar half arcs were used. For NC-VMAT, one full coplanar and two non-coplanar half arcs with couch rotation of 315° or 45°. Dose constraints were adhered to the RTOG0614 and 0933. Dose volumetric parameters were collected for statistical analysis. Results: There were no significant differences for the PTV, HI, CN and μ between the CO-VMAT and NC-VMAT. For the brainstem, Dmean of CO-VMAT and NC-VMAT were 6.04 ± 3.94 Gy and 4.69 ± 2.56 Gy respectively (p < 0.05). For the ipsilateral OARs including temporal lobe, TM joint and cochlear, Dmean of CO-VMAT and NC-VMAT were 31.80 ± 12.78 Gy and 25.51 ± 17.54 Gy (p < 0.01) ; 14.12 ± 8.6 Gy and 3.35 ± 4.12 Gy (p < 0.001); 11.96 ± 11.68 Gy and 6.62 ± 9.74 Gy (p < 0.01) respectively. For contralateral OARs including hippocampus, temporal lobe, TM joint, Optic nerve, lens, eyeball and cochlear, the Dmean of CO-VMAT and NC-VMAT were 6.16 ± 2.44 Gy and 4.49 ± 2.00 Gy (p < 0.01) ; 6.48 ± 2.76 Gy and 3.68 ± 1.76 Gy (p < 0.0001); 11.96 ± 11.68 Gy and 6.62 ± 9.74 Gy (p < 0.01) respectively. Conclusion: The proposed NC-VMAT showed more favourable plan quality than the CO-VMAT for primary brain tumours, in particular to OARs located to the contralateral side-of tumours. Advances in knowledge: For primary brain tumours RT, NC-VMAT can reduce doses to the brainstem, ipsilateral temporal lobe, TM joint and cochlear, as well as OARs located to the contralateral side-of tumours.