Intelligence of living and nonliving systems is often characterized by the ability to communicate through signal and response. In the polymer science community, this intelligence is realized through the reaction of a material construct to environmental triggers. These smart materials are modeled after natural materials, which utilize matrix–fiber architectures to detect stimuli, release small molecules, or alter their macroscopic morphology in response to stimuli. As such, researchers have designed matrix–fiber composites, which function as release vehicles, sensors or switches, and actuators. Through the examination of the architecture and environmental triggering of these natural muses, the fundamental design parameters necessary for functional response in matrix–fiber composites and the ability to utilize these composites in targeted applications are highlighted. Opportunities for innovation in composite design are also discussed.