Regional ecological security assessment is a significant methodology for environmental protection, land utilisation, and human development. This study aims to reveal the regional constraints of ecological resources to overcome the difficulties and complexities in quantification of current models used in land ecosystems. For this purpose, the technique for order preference by similarity to an ideal solution (TOPSIS) was linked to a grey relational analysis and integrated with a geographic information system. The obtained method was used to construct a land eco-security evaluation on a regional scale for application in a traditional mining city, Daye, in central China. Parameter analysis was introduced to the method to produce a more realistic spatial distribution of eco-security. Subsequently, based on the pressure–state–response framework, the eco-security index was calculated, and the carrying capacity of land resources and population for each sub-region were analysed. The results showed that: (i) very insecure and insecure classes comprised 5.65% and 18.2% of the total area, respectively, highlighting the vulnerable eco-environmental situation; (ii) moderate secure classes areas comprised a large amount of arable land, spanning an area of 494.5 km2; (iii) secure areas were distributed in the northwest, containing mostly water and wetland areas and accounting for 426.3 km2; and (iv) very secure areas were located on the southeastern region, involving traditional woodland with a better vegetation cover and an overall higher eco-environmental quality. In addition, for each sub-region, the extremely low and low ecological security areas were mainly arable and urban lands, which amounted to 305 and 190 km2, respectively. Under the current ecological constraints, sub-region 1 cannot continue supporting the population size in Daye City. The present results demonstrate the accuracy of our methodology, and our method may be used by local managers to make effective decisions for regional environment protection and sustainable use of land resources.