Objective To investigate the preparation method, the release profile and structure of the polyelectrolyte layer-by-layer coated chitosan-alginate microgels. Methods The cores of the microgels were prepared by a high voltage electrostatic system, and the semipermeable membrane outside the microgel was polyelectrolyte deposits on the core surface through electrostatic attraction. The influences of different ratios of materials on the expansion property and the in vitro cumulative release of the coated microgels were evaluated by a single factor experiment. Results The prepared polyelectrolyte-coated microgels were well-shaped, with a narrow range of diameter distribution. The lag time of in vitro release was 2.67 h; the release was rapid after lagging, with the cumulative in vitro release being 72% within 3 h. Conclusion Polyelectrolyte layer-by-layer coated chitosan-alginate microgels can release payload in a pulsed fashion in vitro.