New strategies for fabricating multiphase bioceramic porous scaffolds with time-dependent biodegradation and pore network enlargement are of fundamental importance in the advancement of bioceramics. Here, we developed a one-step preparation of core-shell bioceramic microspheres (similar to 2 mm in diameter) with single-or double-shell structure through a coaxially aligned multilayer capillary system. The Ca-phosphate ( CaP) and Ca-silicate ( CaSi) ceramic phase distribution could be also adjusted by extruding through different capillaries, and thus the biodegradation rate would be readily tailored over time. When the polystyrene ( PS) microbeads of similar to 15 mu m in diameter were premixed into the CaP- or CaSi-containing alginate slurry, the tailorable porous structures could be introduced into the core or different shell layers of the microspheres. These micropores may potentially maximize the permeability for rapid exchange of guest molecules or inorganic ions from the bioceramics. Totally, such strategy is promising because the ceramic phases with different biological properties can be assembled into the core-shell bioceramic microspheres, and thus the macropore structure evolution may be readily manipulated in the closely packed microsphere systems. We believe our gradient hybrid methodology will have potential in various categories of advanced biomaterials of organic-inorganic composites.