A coupling membrane process of adsorption-microfiltration for the specific, safe, and effective removal of bilirubin was developed. Chitosan microporous membranes were prepared by template leaching method with silica particles as the leachable component, and equilibrium as well as dynamic adsorption experiments were carried out. The effects of cross-linking processing, adsorption temperature, ion strength, and bilirubin initial concentration on bilirubin clearance were discussed. Results showed that adsorption capacity increases with the increasing of temperature and decreases with the increasing of iron strength. Adsorption mechanism can be well described with Freundlich equation. The adsorption equilibrium can be reached quickly both in static and dynamic experiments, and chitosan membranes have high removal clearance (up to 94%) on bilirubin in phosphate buffer with uncross-linked chitosan membranes, while 84.6% with cross-linked membranes.