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In this study, we investigate the effect of a hierarchically ordered macroporous structure of alumina support on the steam reforming of 1-methyl naphthalene with mesoporous alumina-supported nickel and potassium (xK/Ni–MeAl), and macroporous alumina-supported nickel and potassium (xK/Ni–MaAl) catalysts. Hierarchically ordered macroporosity in Al₂O₃ supports plays an important role in maintaining the high Ni dispersion through multiple interactions in Ni–K over AlO₄ tetrahedra in alumina. This, in turn, improves the catalytic performance of steam reforming, including high gas yields, turnover frequency for hydrogen production, and 1-methyl naphthalene conversion. At high K content, the Ni active sites over xK/Ni–MeAl catalysts significantly decrease, resulting in almost zero steam reforming rate in the reaction test. Conversely, the potassium–alumina interaction in xK/Ni–MaAl catalysts not only diminishes the formation of the inactive nickel aluminate phase but also maintains the highly dispersed Ni active sites, resulting in a high steam reforming rate.