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Modified cokes with improved resistance to CO₂ reaction were produced from a high volatile coking coal (HVC) and different concentrations of boron carbide (B₄C) in a laboratory scale coking furnace. This paper focuses on modification mechanism about the influence of B₄C on coking behavior and chemical structure during HVC carbonization. The former was studied by using a thermo-gravimetric analyzer. For the latter, four semi-cokes prepared from carbonization tests for HVC with or without B₄C at 450 °C and 750 °C, respectively, were analyzed by using Fourier transform infrared spectrum and high-resolution transmission electron microscopy technologies. It was found that B₄C will retard extensive condensation and crosslinking reactions by reducing the amount of active oxygen obtained from thermally produced free radicals and increase secondary cracking reactions, resulting in increasing size of aromatic layer and anisotropic degree in coke structure, which eventually improves the coke quality.