Background: Accumulating evidence has linked environmental exposure, such as ambient air pollution and meteorological factors, to the development and severity of cardiovascular diseases (CVDs), resulting in increased healthcare demand. Effective prediction of demand for healthcare services, particularly those associated with peak events of CVDs, can be useful in optimizing the allocation of medical resources. However, few studies have attempted to adopt machine learning approaches with excellent predictive abilities to forecast the healthcare demand for CVDs. This study aims to develop and compare several machine learning models in predicting the peak demand days of CVDs admissions using the hospital admissions data, air quality data and meteorological data in Chengdu, China from 2015 to 2017. Methods: Six machine learning algorithms, including logistic regression (LR), support vector machine (SVM), artificial neural network (ANN), random forest (RF), extreme gradient boosting (XGBoost), and light gradient boosting machine (LightGBM) were applied to build the predictive models with a unique feature set. The area under a receiver operating characteristic curve (AUC), logarithmic loss function, accuracy, sensitivity, specificity, precision, and F1 score were used to evaluate the predictive performances of the six models. Results: The LightGBM model exhibited the highest AUC (0.940, 95% CI: 0.900-0.980), which was significantly higher than that of LR (0.842, 95% CI: 0.783-0.901), SVM (0.834, 95% CI: 0.774-0.894) and ANN (0.890, 95% CI: 0.836-0.944), but did not differ significantly from that of RF (0.926, 95% CI: 0.879-0.974) and XGBoost (0.930, 95% CI: 0.878-0.982). In addition, the LightGBM has the optimal logarithmic loss function (0.218), accuracy (91.3%), specificity (94.1%), precision (0.695), and F1 score (0.725). Feature importance identification indicated that the contribution rate of meteorological conditions and air pollutants for the prediction was 32 and 43%, respectively.