trade-off between minimized premature

leakage and rapid cargo release on demand is an intractable

obstacle faced by smart delivery systems that restrains them

from lab to market. To address this dilemma, dynamic hybrid

colloidosomes relying on strong yet reversible electrostatic

interactions are developed, simply through one-pot cooperative

self-assembly of silica nanoparticles and fluorescent

carbon dots at the interface of emulsion droplets. Specifically,

pH-driven charge reversal of zwitterionic carbon dots leads to

immediate electrostatic conversion between the two building blocks from attraction to repulsion. This makes robust locking and

instantaneous breakdown of the colloidosomes subtly balanced, thus enabling low off-state leakage (10.5% over 7 days) while

ultrafast on-state release (>90% within 5 min) upon an acidic stimulus. We envision that such biocompatible, traceable, and

smart colloidosomes will offer unique opportunities for broad applications as on-demand release is desired.