A new approach is reported on the use of poly(Nisopropylacrylamide) (PNIPAM)-coated molecularly imprinted beads (coated MIP beads) for controlling the release of protein. The coated MIP beads were composed of double layers, an internal thermosensitive lysozymeimprinted layer, and an external PNIPAM layer. The coated MIP beads were prepared by two-step surface-initiated living-radical polymerization (SIP). In this systemic study, the coated MIP beads had good selectivity to the template protein (lysozyme) and temperature stimulus-responsive behavior, both of which were superior to those of MIP beads having a layer of thermosensitive lysozyme-imprinted polymer only. Using the coated MIP beads, reference proteins and the template lysozyme could be released separately at 38°C and at 23°C. The corresponding coated non-imprinted beads (coated NIP beads) did not have such double thermosensitive "gates" with specific selectivity for a particular protein. The proposed smart controlled imprinted system for protein is attractive for chemical carriers, drugdelivery system, and sensors.