To explore the predictive value of absolute and relative iodine concentrations in the spot sign (SS) and haematoma on gemstone spectral imaging (GSI) for haematoma expansion (HE). Patients with spontaneous intracerebral haemorrhage (ICH) who underwent computed tomography (CT) angiography using GSI were divided into an SS-positive group and an SS-negative group. In the SS-positive group, absolute and relative iodine concentrations in the SS (aICIS and rICIS, respectively) were measured. In the SS-negative group, absolute and relative iodine concentrations in haematoma (aICIH and rICIH, respectively) were measured. The area under the receiver operating characteristic curve (AUC-ROC) was used to investigate the HE predictive performance of aICIS, rICIS, and their combination in the SS-positive group, as well as the HE predictive performance of aICIH, rICIH, and their combination in the SS-negative group. The risk variables for HE in the two groups were investigated separately using logistic regression. A total of 123 spontaneous ICH patients were enrolled. In the SS-positive group, the AUC of aICIS, rICIS, and their combination for predicting HE were 0.853, 0.893, and 0.922, respectively. rICIS was demonstrated to be a standalone predictor of HE via logistic regression. In the SS-negative group, aICIH, rICIH, and their combination had AUC-ROC values of 0.552, 0.783, and 0.851, respectively, to predict HE. According to multivariate analysis, rICIH was a reliable predictor of HE. Absolute and relative iodine concentrations in the SS and haematoma can predict HE.