1. Leaf-litter ants represent a major component of biodiversity and are excellent bioindicators reflecting the health of terrestrial ecosystems. This study, conducted in an unspoiled forest near the Nouragues Research Station, represents the first inventory of leaf-litter ant diversity conducted in French Guiana, and so can be considered as the baseline dataset for ants in this country. 2. Ants were extracted from the leaf-litter using the Ants of the Leaf Litter Protocol, along an altitudinal gradient at four forest sites, including an inselberg. 3. A total of 196 ant species representing 46 genera distributed over eight subfamilies were collected. Four distinct communities spread over a gradient of diversity were thus identified: the liana forest was the most species-rich (140 species) followed by the forested plateau (102 species), the transition forest (87 species) and the forest at the top of the inselberg (71 species). 4. The discovery of species new to science plus several species recorded for the first time in French Guiana, coupled with the particular context of this area, suggests that the Nouragues Research Station might represent a centre of endemism. Once completed, this leaf-litter ant dataset will contribute greatly to the knowledge of ant biodiversity in French Guiana, and has the potential to progressively become an indispensable tool for country-wide conservation planning programmes.