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Background: Preoperative prediction of postoperative pulmonary function after anatomical resection for lung cancer is essential to prevent long-term morbidity and mortality. Here, we compared the accuracy of hybrid single-photon emission computed tomography/computed tomography (SPECT/CT) with traditional anatomical and planar scintigraphy approaches in predicting postoperative pulmonary function in patients with impaired lung function. Methods: We analyzed the predicted postoperative pulmonary function in patients undergoing major anatomical lung resection, applying a segment counting approach, planar perfusion scintigraphy (PPS), and SPECT/CT-based lung function quantification. Results: In total, 120 patients were evaluated, of whom 82 were included in the study. Postoperative lung function tests were obtained in 21 of 82 patients. The preoperative SPECT/CT-based quantification yielded very accurate results compared to the actual postoperative FEV1 and DLCO values. The linear regression analysis showed that the SPECT/CT-based analysis predicted postoperative FEV1 (%) and DLCO values more accurately than the segment counting approach or PPS. Accordingly, 58/82 patients would qualify for anatomical lung resection according to the SPECT-based quantification, 56/82 qualified according to the PPS (Mende), and only 47/82 qualified according to the segment counting method. Moreover, we noted that the SPECT-predicted FEV1 values were very close to the actual postoperative values in emphysema patients, and selected patients even showed improved lung function after surgery. Conclusions: Anatomically driven methods such as SPECT/CT yielded a very accurate prediction of the postoperative pulmonary function. Accordingly, applying SPECT/CT revealed more patients who would formally qualify for lung resection. We suggest SPECT/CT as the preferred method to evaluate eligibility for lung surgery in selected patients with impaired pulmonary reserve. [ABSTRACT FROM AUTHOR]