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Background: Patients with severe stroke are at high risk of secondary neurologic decline (ND) from the development of malignant cerebral edema (MCE). However, early infarcts are hard to diagnose on conventional head computed tomography (CT). We hypothesize that high-energy (190 keV) virtual monochromatic imaging (VMI) from dual-energy CT (DECT) imaging enables earlier detection of ND from MCE., Methods: Consecutive patients with severe stroke with National Institute of Health Stroke Scale (NIHSS) scores > 15 and DECT within 10 h of mechanical thrombectomy from May 2020 to March 2022 were included. We excluded patients with parenchymal hematoma type 2 transformation. Retrospective analysis of clinical and novel variables included the VMI Alberta Stroke Program Early CT Score (ASPECTS), total iodine content, and VMI infarct volume. The primary outcome was secondary ND, defined using a composite outcome variable of clinical worsening (increase in NIHSS score ≥ 4 or decrease in Glasgow Coma Scale score > 2) or malignant radiographical edema (midline shift ≥ 5 mm at the level of the septum pellucidum). Fisher's exact test and Wilcoxon's test were used for univariate analysis. Logistic regression was used to develop prediction models for categorical outcomes., Results: Eighty-four patients with severe stroke with a median age of 67.5 (interquartile range [IQR] 57-78) years and an NIHSS score of 22 (IQR 18-25) were included. Twenty-nine patients had ND. The VMI ASPECTS, total iodine content, and VMI infarct volume were associated with ND. The VMI ASPECTS, VMI infarct volume, and total iodine content were predictors of ND after adjusting for age, sex, initial NIHSS score, and tissue plasminogen activator administration, with areas under the receiver operating characteristic curve (AUROC) of 0.691 (95% confidence interval [CI] 0.572-0.810), 0.877 (95% CI 0.800-0.954), and 0.845 (95% CI 0.750-0.940). By including all three predictors, the model achieved an AUROC of 0.903 (95% CI 0.84-0.97) and was cross-validated by the leave one out method, with an AUROC of 0.827., Conclusions: The VMI ASPECTS and VMI infarct volume from DECT are superior to the conventional CT ASPECTS and are novel predictors for secondary ND due to MCE after severe stroke. Clinical trial registration ClinicalTrials.gov identifier: NCT04189471., (© 2024. Springer Science+Business Media, LLC, part of Springer Nature and Neurocritical Care Society.)