Arthropods are traditionally viewed as invertebrate prey and predators for vertebrates, a paradigm increasingly challenged, especially among arachnids. While spiders are documented frog predators, the capacity of other groups like harvestmen (Opiliones) has remained anecdotal. We report novel field observations of anuran predation by multiple Cranaidae harvestmen species across Neotropical localities. These records include active capture and consumption of live frogs, demonstrating their role as opportunistic mesopredators. Alongside new spider predation records, our findings substantially advance Opiliones ecology by confirming vertebrate predation occurs in multiple, disjunct species. This reveals vertebrate consumption among arachnids is more taxonomically widespread than recognized, underscoring the need to include Opiliones as potential predators in Neotropical trophic models.