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A pedogeochemical exploratory survey of gold deposits was carried out in the region of São Sepé (southernmost Brazil). The region comprises a predominantly metamorphosed belt of volcanoclastics, sediments, serpentinites, basalts, gabbros, chert, tuffs, and banded iron formation of the Proterozoic age. The anomalies were identified first by stream sediment heavy mineral survey at the regional scale of exploration. Once spatial continuity was modeled, ordinary block kriging was performed to generate geochemical maps. Indicator block kriging also was used as an alternative in analyzing and interpreting geochemical data. A novel approach is proposed, which combines both ordinary and indicator kriging for delineating geochemical anomalies. Probability maps proved to be appropriate for selecting new sites for further exploration. Gold anomalies in soils trending NE were well defined by geostatistical analysis and subsequently confirmed by drilling.