We have previously reported on a method for reconstructing quantitative data from 99mTc single photon emission computed tomography (SPECT) images based on corrections derived from X-ray computed tomography, producing accurate results in both experimental and clinical studies. This has been extended for use with the radionuclide ²⁰¹Tl. Accuracy was evaluated with experimental phantom studies, including corrections for partial volume effects where necessary. The quantitative technique was used to derive standardized uptake values (SUVs) for ²⁰¹Tl evaluation of brain tumours. A preliminary study was performed on 26 patients using ²⁰¹Tl SPECT scans to assess residual tumor after surgery and then to monitor response to treatment, with a follow-up time of 18 months. Measures of SUVmax were made following quantitative processing of the data and using a threshold grown volume of interest around the tumour. Phantom studies resulted in the calculation of concentration values consistently within 4% of true values. No continuous relation was found between SUVmax (post-resection) and patient survival. Choosing an SUVmax cut-off of 1.5 demonstrated a difference in survival between the 2 groups of patients after surgery. Patients with an SUVmax<1.5 had a 70% survival rate over the first 10 months, compared with a 47% survival rate for those with SUVmax>1.5. This difference did not achieve significance, most likely due to the small study numbers. By 18 months follow-up this difference had reduced, with corresponding survival rates of 40% and 27%, respectively. Although this study involves only a small cohort, it has succeeded in demonstrating the possibility of an SUV measure for SPECT to help monitor response to treatment of brain tumours and predict survival.