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Optimization of continuous synthesis of high purity carbon nanotubes (CNTs) using chemical vapour deposition (CVD) method was studied experimentally and theoretically. Iron pentacarbonyl (Fe(CO)5), acetylene (C2H2) and Ar were used as the catalyst source, carbon source and carrier gas respectively. The synthesis temperature and flow rates of Ar and acetylene were optimized to produce CNTs at a large scale. A flow rate of 30-120 sccm of acetylene and 500-3000 sccm of Ar at temperatures between 650-950 °C were examined. Using the fundamental trial and error method it was found that the maximum yield of pure CNTs can be produced at 750 °C with flow rates of 40-45 sccm of acetylene and 1500 sccm of Ar. In theoretical part, an artificial neural network (ANN) and the Bees Algorithm (BA) were used to model and optimize the CNTs production, based on the experimental data. The Bees Algorithm used the ANN as the fitness function and the optimum variables found as 60 sccm for acetylene, 555 sccm for argon and 759 °C for temperature. The computational results have relatively good agreement with the experimental results.