Exogenous carbon addition is widely regarded as an effective soil management strategy for rapidly increasing soil organic carbon, improving soil structure and function. However, a systematic comparison of the effects of diverse organic amendments on key soil attributes and processes is needed to inform their targeted application. We evaluated the impacts of seven organic amendments (biochar, organic fertilizer, corn straw, soybean straw, rapeseed straw, green manure, and carbon material) on a purple soil (Luvic Xerosols) in a pot experiment. The results showed that organic fertilizer and carbon material performed best in enhancing soil nutrient availability and promoting soil organic carbon content. Straw amendments promoted the formation of macro-aggregates. Green manure and straws enhanced carbon transformation-related β-glucosidase and cellobiohydrolase activities. Random Forest and structural equation modeling indicated that the organic amendments enhanced maize carbon sequestration capacity and biomass by improving aggregate stability and regulating the fungal community and by increasing nutrients and enhancing active carbon fractions. Green manure and organic fertilizer demonstrated the most significant agronomic effects. These findings provide guidelines for targeted organic amendment selection in purple soil regions.