Stimuli-responsive gate mechanisms offer potential for the controlled passage of payload molecules from a porous carrier vehicle on-demand. We describe a method for the enzyme-mediated release of macromolecular guest molecules from inorganic silica particles coated with a bioactive peptide shell, synthesized precisely by Fmoc chemistry. Specific enzymatic hydrolysis of the peptide shell removes the bulky peptide-terminated Fmoc groups, permitting the selective release of previously entrapped guest molecules.