Appraisals of land-use sustainability (LUS) are indispensable for the attainment of sustainable land-use planning and management. At present, China is experiencing a pivotal phase of comprehensive reform in land-use policy, engendering a practical necessity for system-oriented land evaluations. Despite this, studies focused on national-scale systematic LUS evaluation remain scarce. Within this context, we developed a hierarchical structural framework for land-use systems based on the assumption that sustainable land-use systems adapted to development needs have mutually adaptable internal subsystems and fewer conflicting system elements. Employing this framework, we assessed the LUS across Chinese counties from 2000 to 2015 by using a newly introduced static equilibrium equation;we also analyzed the natural and socioeconomic influences and driving effect of land-use change to LUS. Findings reveal a significant spatial clustering and urban-rural differentiation within the LUS spatial pattern. Five LUS hot and cold spots and eight metropolitan areas with poor LUS were identified. Furthermore, conflicting land capability elements and the non-adaptability of land function subsystems with capability subsystems are the primary constraints on LUS; gross domestic product (GDP), population growth, and the GDP growth per unit land area had the most significant impacts on LUS; The transformation of construction and cropland into ecological land and the re-purposing of grassland into building land are primary drivers of LUS. Our findings highlight the prospective utility of the proposed LUS framework in integrated natural resource management and territorial spatial planning. Meanwhile, Insights from this evaluation case could be harnessed to optimize land-use in critical regions (including northern arid and semiarid regions, the Qinghai–Tibet Plateau region, the poverty belt around the capital, Yangtze River Delta and Pearl River Delta metropolitan areas, as well as Fuzhou and Xiamen metropolitan areas), thereby enhancing land management decision-making processes.