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In this study, the effects of coal blending ratio, pyrolysis temperature, pyrolysis atmosphere and coal particle size on the quality of pyrolyzed char were investigated via a combination of orthogonal experimental design and grey relational analysis. Coal-XG and Coal-LL were pyrolyzed under various conditions to produce chars which were characterized to ascertain their properties such as chemical structure and reactivity. The results indicated that the pyrolysis temperature has the most significant impact on the quality of the char, followed by the pyrolysis atmosphere, coal blending ratio and coal particle size. The increase in pyrolysis temperature not only diminished char yield but also accelerated the consumption of oxygen-containing functional groups and the polycondensation of small aromatic ring structures throughout the reaction process. This led to a reduction in the reactivity of pyrolyzed char and the establishment of a more ordered structure. Meanwhile, the involvement of CO 2 and H 2 O prevented the condensation of small aromatic rings and fostered the generation of additional oxygen-containing functional groups, which resulted in lower yield and higher reactivity of the char under these two atmospheres. Through systematic analysis, only the Raman characteristic parameter I (Gr+VL+Vr) /I D exhibited a strong positive linear correlation with char reactivity, making it a reliable indicator for characterizing the reactivity of char. • The orthogonal design was used to study four response factors. • GRA was used to find optimal conditions and impact ranking of different factors. • Linear regression was applied to relate Raman/FTIR parameters to reactivity. • Blend experiments were conducted with two coking coals. [ABSTRACT FROM AUTHOR]