The chemical control of cell division has attracted much attention in the areas of single cell-based biology and high-throughput screening platforms. A mussel-inspired cytocompatible encapsulation method for achieving a cell-division control with cross-linked layer-by-layer (LbL) shells is developed. Catechol-grafted polyethyleneimine and hyaluronic acid are chosen as polyelectrolytes for the LbL process, and the cross-linking of polyelectrolytes is performed at pH 8.5. Cell division is controlled by the number of the LbL nanolayers and cross-linking reaction. We also suggest a new measuring unit, t-2.0 OD 600, for quantifying cell-division timing based on microbial growth kinetics.