Cocoa products and chocolate have recently been recognized as a rich source of flavonoids, mainly flavanols, potent antioxidant and anti-inflammatory agents with established benefits for cardiovascular health but largely unproven effects on neurocognition and behavior. In this review, we focus on neuromodulatory and neuroprotective actions of cocoa flavanols in humans. The absorbed flavonoids penetrate and accumulate in the brain regions involved in learning and memory, especially the hippocampus. The neurobiological actions of flavanols are believed to occur in two major ways: (i) via direct interactions with cellular cascades yielding expression of neuroprotective and neuromodulatory proteins that promote neurogenesis, neuronal function and brain connectivity, and (ii) via blood-flow improvement and angiogenesis in the brain and sensory systems. Protective effects of long-term flavanol consumption on neurocognition and behavior, including age- and disease-related cognitive decline, were shown in animal models of normal aging, dementia, and stroke. A few human observational and intervention studies appear to corroborate these findings. Evidence on more immediate action of cocoa flavanols remains limited and inconclusive, but warrants further research. As an outline for future research on cocoa flavanol impact on human cognition, mood, and behavior, we underscore combination of functional neuroimaging with cognitive and behavioral measures of performance.