Benthic cyanobacterial mats (BCMs) are conspicuous components of coral reef communities, where they play key ecological roles as primary producers among others. BCMs often bloom and might outcompete neighboring benthic organisms, including reef-building corals. We investigated the cyanobacterial species composition of three BCMs morphotypes from the marginal reef complex of Abrolhos Bank (Southeastern Brazil). Also, we assessed their allelopathic effects on coral zooxanthellae, their susceptibility to herbivory by fish, and their toxicity to brine shrimp nauplii. Morphology and 16S rDNA sequencing unveiled the cyanobacteria Moorena bouillonii, Okeania erythroflocculosa, Adonisia turfae, Leptolyngbya sp., and Halomicronema sp. as components of BCMs from Abrolhos. BCMs cell-free filtrates and extracts exerted an allelopathic effect by reducing the growth of the ex hospite Symbiodinium sp. in culture. BCMs-only treatments remained untouched in field susceptibility assays in contrast to macroalgae only and mixed BCMs-macroalgae treatments that had the macroalgae fully removed by reef fish. Crude aqueous extracts from BCMs were toxic to brine shrimps in acute assays. Besides unveiling the diversity of BCMs consortia in Abrolhos, our results cast some light on their allelopathy, antiherbivory, and toxicity properties. These antagonistic interactions might promote adverse cascading effects during benthic cyanobacteria blooms and in gradual shifts to BCMs-dominated states.