Aims <p>To address the serious environmental concerns caused by the accumulation of coal gangue from coal mining and fill the research gap in transforming coal gangue into soil-like substrates, this study aims to explore the feasibility of converting coal gangue into soil-like substrates via the combination of organic amendment and plant colonization.</p> Methods <p>Coal gangue-based soil-like substrates were cultivated through pot experiments. The basic physicochemical properties, mineral composition, functional group characteristics, aggregate content and stability, pore structure, and microbial community composition of the substrates were systematically characterized.</p> Results <p>Organic amendment and plant colonization did not alter the primary crystalline phases of coal gangue, but promoted surface Fe oxidation, Fe chemical-state transformation, oxygen-containing functional group enrichment, and reactive Fe/Al accumulation. These changes enhanced organo–mineral associations, facilitating aggregate formation and stability. Pore structure was also optimized, with increased medium and large pores. The improved microenvironment further promoted bacterial community restructuring and enhanced microbial network complexity.</p> Conclusion <p>The combined application of organic amendment and plant colonization represents a feasible technical strategy for promoting the soil-like development of coal gangue substrates. Coal gangue amelioration is a coupled process involving mineral surface activation, physical structural reconstruction, and microbial community succession. These findings provide a mechanistic basis for transforming coal gangue, a mining waste with mild chemical constraints but poor physical structure, into a functional soil-like substrates.</p>