Gymnotus is the most species-rich and geographically widespread genus of gymnotiform electric fishes and has been widely explored to understand mechanisms of diversification in Neotropical freshwater fishes at a continental scale. Within Gymnotus, the subgenus Lamontianus is a phenotypically distinctive clade with an elongate, cylindrical body shape currently known from four valid species (G. anguillaris, G. cataniapo, G. pedanopterus, and G. tiquie) restricted to rivers draining the Guiana Shield. Here we use aspects of body-surface coloration, meristic, morphological, and osteological data, including cranial, laterosensory pore, and postcranial characters, to diagnose two new species of Lamontianus that inhabit the Aripuanã and Arapiuns rivers that drain the Brazilian Shield. We also use geometric morphometric analyses of head shape to separate the new species from one another and other species of Lamontianus. We report biogeographic distributions for all species of Lamontianus and estimate ancestral geographic ranges and range evolution using the parametric biogeographic program BioGeoBEARS. We use the phylogeny of Lamontianus to test alternative hypotheses regarding lineage divergence times, before or after the formation of the modern East-draining Amazon at c. 10 Ma. Our analysis suggests that diversification in Lamontianus occurred primarily by geographic range fragmentation (vicariance) from an ancestral species distributed across the Western Guiana Shield. These results are similar to those of other Gymnotus and gymnotiform clades, where allopatric speciation and secondary contact due to geographic range expansion are commonly observed. This study brings to 46 the number of valid species of the genus Gymnotus, and to six the number of valid species of the subgenus Lamontianus.