In this study, an artificial neural network model using function fitting neural networks was developed to describe the yield and quality of multi-walled carbon nanotubes deposited over NiMo/CaTiO3 catalyst using waste polypropylene plastics as cheap hydrocarbon feedstock using a single-stage chemical vapour deposition technique. The experimental dataset was developed using a user-specific design with four numeric factors (input variable): synthesis temperature, furnace heating rate, residence time, and carrier gas (nitrogen) flow rate to control the performance (yield and quality) of produced carbon nanotubes. Levenberg–Marquardt algorithm was utilized in training, validating, and testing the experimental dataset. The predicted model gave a considerable correlation coefficient (R) value close to 1. The presented model would be of remarkable benefit to successfully describe and predict the performance of polypropylene-derived carbon nanotubes and show how the predictive variables could affect the response variables (quality and yield) of carbon nanotubes.