We provide the first known documentation of a fatal brown bear (Ursus arctos) poisoning with carbofuran (an acetylcholinesterase inhibitor) in Croatia. Diagnosis using liquid chromatography–mass spectrometry confirmed the presence of high concentrations of carbofuran in liver and kidney tissue (12.650 and 2.695 ppm, respectively). These measurements, combined with the very small distance between poisonous baits and the brown bear carcass, provided the basis on which we concluded that the animal consumed a lethal dose of carbofuran and succumbed to acute poisoning soon thereafter. We believe this mortality was caused by the illegal placement of this poison probably to eliminate perceived pests, such as jackals (Canis aureus) or foxes (Vulpes vulpes). Our documentation may help identify similar cases and raise awareness of the risks posed by illegal poisons for non-target species, particularly scavengers such as bears.