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Psychological distress in primary malignant brain tumour (PMBT) patients is associated with poorer outcomes. Radiotherapy (RT) often induces side effects that significantly influence patients’ quality of life (QoL), with potential impact on survival. We evaluated distress, anxiety, depression, and QoL over time to identify patients with difficulties in these areas who required more intense psychological support. Psychological questionnaires—Distress Thermometer (DT), Hospital Anxiety and Depression Scale (HADS), and Functional Assessment of Cancer Therapy (FACT-G and FACT-Br)—were completed at the beginning (T0), in the middle (T1), directly after RT (T2), and 3 months after RT (T3). We personalised the psychological support provided for each patient with a minimum of three sessions (‘typical’ schedule) and a maximum of eight sessions (‘intensive’ schedule), depending on the patients’ psychological profiles, clinical evaluations, and requests. Patients’ survival was evaluated in the glioblastoma multiforme (GBM) patients, with an explorative intent. Fifty-nine consecutive PMBT patients receiving post-operative RT were included. For patients who were reported as ‘not distressed’ at T0, no statistically significant changes were noted. In contrast, patients who were ‘distressed’ at T0 showed statistically significant improvements in DT, HADS, FACT-G, and FACT-Br scores over time. ‘Not distressed’ patients required less psychological sessions over the study duration than ‘distressed’ patients. Interestingly, ‘not distressed’ GBM patients survived longer than ‘distressed’ GBM patients. Increased psychological support improved distress, mood, and QoL for patients identified as ‘distressed’, whereas psychological well-being was maintained with typical psychological support in patients who were identified as being ‘not distressed’. These results encourage a standardisation of psychological support for all RT patients.