Elevated arsenic (As) concentrations in soil are often found in the vicinity of certain mineral deposits that have been, or are currently, under exploitation, regardless of the target resource. Detailed study of such areas for safe agriculture requires considerable financial costs and long periods of time. Application of an appropriate spatial model that describes the behavior of arsenic in soil and plants can significantly ease the whole investigation process. This paper presents a model of ecological security of an area that, in the past, was an antimony mine and has a naturally high content of arsenic. For simulation and modeling the geographic information science (GIS) technology with the inserted predictors influencing the accessibility of As and its content in plants was used. The results obtained were the following: (1) a categorization of contaminated soils according to soil properties was developed; (2) the proposed methodology allows focusing on particular suspect area saving an energy and human resource input; and (3) new safe areas for growing crops in contaminated area were modeled. The application of the proposed model of As solubility to various crops grown around a former antimony mine near the village of Lisa, southwest Serbia showed that significant expansion of the areas suitable for growing potato, raspberry, and pasture was possible.