Abstract: Sustainable intensification of cropland use represents a viable approach to mitigating food security challenges and alleviating environmental pressures. By comprehensively examining material inputs, desirable outputs, and undesirable outputs, this paper constructed an evaluation framework for the sustainable intensification of cropland use. In addition, by integrating the Super-SBM model, Dagum Gini coefficient, and the GTWR method, this paper analyzed the spatiotemporal evolution, regional disparities, typological patterns, and optimization strategies of sustainable intensification levels across 86 counties in Hunan Province from 2000 to 2021. The results indicate that temporally, the level of sustainable intensification of cropland in Hunan’s counties showed a phased upward trend, characterized by an evolutionary process of “decline-adjustment-rise”. Spatially, high-value areas exhibited a diffusion pattern from the northeastern and southwestern regions toward the central area, medium-value areas demonstrated significant agglomeration with a “lock-in effect”, and low-value areas were concentrated in the western part. In terms of regional disparity, overall inequality displayed a declining trend, largely driven by inter-regional differences, while intra-regional differences remained relatively small and stable, indicating a “balanced steady-state effect”. The driving mechanisms were influenced by natural, economic, demographic, and policy factors, with spatiotemporal heterogeneity in the effects of these drivers. Eight typical driving patterns were identified, suggesting that region-specific and time-aware differentiated pathways should be formulated to promote sustainable intensification of cropland use. The findings aim to provide insights for facilitating sustainable agricultural intensification and enhancing agricultural modernization in various regions.