Spatially controlled confinement of catalytic enzymes within nanoshells holds substantial potential for applications in bioreactors, synthetic cells, and artificial spores. The utilization of amorphous calcium phosphate (CaP) precursors enables the extremely rapid (<5 seconds) construction of thick (∼400 nm) CaP nanoshells, stratified with distinct enzymes, on various tannic acid-primed substrates. Saccharomyces cerevisiae cells are nanoencapsulated with enzyme-embedded, multilayered CaP nanoshells in a cytocompatible manner, providing an advanced chemical tool for interfacing living cells with functional entities in a spatially controlled configuration.