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The harm done to the environment by coal gangue was very serious, and it is urgent to adopt effective methods to dispose of coal gangue in order to prevent further environmental damage. Co-pyrolysis experiments of coal gangue (CG) and peanut shell (PS) were carried out using thermogravimetry-Fourier transform infrared spectroscopy (TG-FTIR) under nitrogen atmosphere. The heavy metal was detected using the inductively coupled plasma-optical emission spectroscopy (ICP-OES). CG and PS were mixed according to the mass ratio of 1:0, 3:1, 1:1, 1:3 and 0:1. The samples were heated to 1000 °C at the heating rate of 10 °C/min, 20 °C/min and 30 °C/min. The comprehensive pyrolysis index (CPI) of CG, C3P1, C1P1, C1P3 and PS is 0.17 × 10−8, 9.75 × 10−8, 35.47 × 10−8, 100.94 × 10−8 and 192.72 × 10−8%2 ·min−2·°C−3. The kinetic parameters were calculated by model-free methods (Flynn–Wall–Ozawa and Kissinger–Akahira–Sunose). The gas products generated at different temperatures during the pyrolysis experiment were detected by Fourier transform infrared spectrometer. The heating rate, temperature and mixing ratio are the input parameters of artificial neural network (ANN), and the remaining mass percentage of sample during the pyrolysis is the output parameter. The ANN model was established and used to predict thermogravimetric experimental data. The ANN18 model is the best model for predicting the co-pyrolysis of CG and PS. Unlabelled Image • First study on application of ANN model to co-pyrolysis of CG and PS • Synergistic effect between CG and PS was found during C3P1 and C1P3 co-pyrolysis. • The TG-FTIR was used to detect the functional groups of gas during pyrolysis. • Activation energy was estimated from the KAS and FWO methods. • The ultimate goal of this study is to reduce environmental pollution caused by CG. [ABSTRACT FROM AUTHOR]