New finds of Hyolitha in the Devonian of Bolivia consist of the hyolithid Bolithes crasquinae new genus and species, which is the first well-preserved hyolithid from strata of this age in the region. In addition, specimens of the orthothecids Bolitheca steinmanni (Knod, 1908) and Neobactrotheca pharetra Marek and Isaacson, 1992 serve to increase knowledge concerning the range of morphologic variability within those taxa. Incompletely preserved hyoliths include Hyolithes sp. indet.? which would be the first definitive representative of that genus from South America. Two polyclaviculate hyolithid opercula, and an unusually large hyolithid conch are left in open nomenclature. The large conch is noteworthy because of signs of failed predation, making this only the second hyolithid on record on which the effects of predation can be recognized, and the first from the Devonian of South America. Hyolithes dorbignyi Kozlowski, 1923 is transferred to ‘Hyolithes’ owing to poor preservation.