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Single‐cell nanoencapsulation, forming cell‐in‐shell structures, provides chemical tools for endowing living cells, in a programmed fashion, with exogenous properties that are neither innate nor naturally achievable, such as cascade organic‐catalysis, UV filtration, immunogenic shielding, and enhanced tolerance in vitro against lethal factors in real‐life settings. Recent advances in the field make it possible to further fine‐tune the physicochemical properties of the artificial shells encasing individual living cells, including on‐demand degradability and reconfigurability. Many different materials, other than polyelectrolytes, have been utilized as a cell‐coating material with proper choice of synthetic strategies to broaden the potential applications of cell‐in‐shell structures to whole‐cell catalysis and sensors, cell therapy, tissue engineering, probiotics packaging, and others. In addition to the conventional “one‐time‐only …