Among diflerent synthetic platforms, mesoporous silica-based materials have gainedmuch attention in many potential nanotechnology areas (such as optoclectronics[l],catalysis[2], or sensing[3J). In particular, they have set a precedent in the area ofnanomcdicinc as dmg delivery systems[4]. Their thermal stability, a rigid framework whichprevents premature degradation of the cargo, and their easy chemical attachment of responsiveunits that exhibit a control over undesirable uncspccific release[5J. arc fcnturcH that mak«sthem stand out candidates. The external functionalization with stimuli-rcsponsivc gate-keeperunits by post-grafting strategy (Figure l.a) allows a control release upon application ofdifferent stimuli. Hence, we designed different hybrid molecular gate-like nanomaterialscontaining pH. temperature or light-sensitive organic functionalities to control the release ofchcmotherapcutics through a selective i€close-opcning gate mechanism" (Figure l.b) underpathological conditions typical of cancer cells.