In order to improve the combustion efficiency and decomposition rate of the cement calciner and reduce pollutant emission, a performance optimization method based on Computational Fluid Dynamics (CFD) numerical simulation integrated with machine learning is proposed. The Multiphase Particle-in-cell (MP-PIC) method and the chemical reaction models are employed to simulate the coal combustion and CaCO3 decomposition process, whose calculation results are combined with the industrial practical data of the cement plant, so as to establish a more comprehensive training database. On this basis, a novel Topology Particle Swarm Optimization algorithm integrating with Convolutional Neural Network and Long Short-Term Memory (RITPSO–CNN–LSTM) algorithm model is established to predict combustion efficiency, decomposition rate, and NOx emission, respectively. Results show that compared with two other relative basic algorithm models, the prediction error of the proposed algorithm model for the three targets is minimal with the average relative error of 0.045 %, 0.038 %, and 0.021 %, respectively. The addition of CFD simulation data makes the prediction model more applicable with higher stability and accuracy. Based on the prediction results, Grey Wolf Optimizer (GWO) algorithm is employed to optimize operating parameters, and finally the average optimization amount of combustion efficiency, decomposition rate, and NOx emission are 2.17 %, 2.24 %, and 6.15 ppm, respectively, which meet the optimization requirements.