In recent years, colorimetric biosensing has attracted much attention because of its low cost, simplicity, and practicality. Since color changes can be read out by the naked eye, colorimetric biosensing does not require expensive or sophisticated instrumentation and may be applied to field analysis and point-of-care diagnosis. For transformation of the detection events into color changes, a number of smart materials have been developed, including gold nanoparticles, magnetic nanoparticles, cerium oxide nanoparticles, carbon nanotubes, graphene oxide, and conjugated polymers. Here, we focus on recent developments in colorimetric biosensing using these smart materials. Along with introducing the mechanisms of color changes based on different smart materials, we concentrate on the design of biosensing assays and their potential applications in biomedical diagnosis and environmental monitoring.