The presence of complementary information across multiple sensory or motor modalities during learning, referred to as multimodal enrichment, can markedly benefit learning outcomes. Why is this? Here, we integrate cognitive, neuroscientific, and computational approaches to understanding the effectiveness of enrichment and discuss recent neuroscience findings indicating that crossmodal responses in sensory and motor brain regions causally contribute to the behavioral benefits of enrichment. The findings provide novel evidence for multimodal theories of enriched learning, challenge assumptions of longstanding cognitive theories, and provide counterevidence to unimodal neurobiologically inspired theories. Enriched educational methods are likely effective not only because they may engage greater levels of attention or deeper levels of processing, but also because multimodal interactions in the brain can enhance learning and memory.