Hydroxyapatite/chondroitin sulfate (HAp/ChS) microparticles with the perfectly spherical shape and the averaged particle sizes of 4.1, 7.8, 19.9 and 29.4 µm were fabricated by a spray dry method under the different atomizing pressures and the concentrations of suspensions. The contents of ChS in the microparticles were varied at 1.49, 3.18, 7.82, 14.2 wt%, and the ChS elution rate in distilled water from the microparticles was increased with the increase of ChS contents. The adsorption isotherms of cytochrome C on the microparticles in 1/10 diluted phosphate buffer saline (PBS) were followed to the Langmuir’s equation regardless of the change of ChS contents, while those of catalase were not followed. The HAp/ChS microparticles can adsorb greater amount of cytochrome C than pure HAp microparticles, but less amount of catalase than pure HAp. The electrostatic interaction between the proteins and ChS was of great importance in the adsorption properties.