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Harvesting, training, and domesticating living organisms to apply their intrinsic capabilities to desired applications is one of the most fundamental of human accomplishments. Extending this concept to the cellular level requires precise control of the chemical interface between live cells and synthetic materials. One great challenge is to progress from empirically surveying cellular behaviors to the predictive design of synthetic substrates that communicate specific signals to cells. This requires a detailed understanding of cell signaling mechanisms as well as the ability to synthesize hybrid materials that incorporate biological molecules in precisely defined ways. A number of promising advances in the development of synthetic interfaces with cells suggest that the move to predictive design is under way.