Biomineralized polysaccharide-coated alginate beads containing PNIPAAM were prepared. The resulting beads can be used as carriers for sustained pH/temperature-sensitive drug delivery. Characterizations using SEM, EDS, FTIR, and POM revealed that the beads were covered by the calcium-phosphate-mineralized alginate/chitosan membrane. The drug-release behavior was examined using indomethacin as a model drug, and the release profile of the developed materials was found to be responsive to pH and temperature. The release profile could be sustained under neutral conditions, indicating that the mineralized polysaccharide membrane could prevent the permeability of the encapsulated drug and reduce the drug release rate.