Stable surfactant-free, water-dispersed, micron-sized organic solvent colloids have been a challenging subject of major interest both experimentally and theoretically in recent years. In this article, novel matrix capsules are introduced to carry an organic solvent ( toluene) into water and form a stable solvent dispersion in the aqueous phase without the addition of a surfactant. The structure and dynamics of the dispersion are investigated by confocal Raman microscopy, surface force microscopy, and pulsed field gradient nuclear magnetic resonance (PFG-NMR). The matrix capsules are fabricated according to a literature method using alternating layer-by-layer adsorption of oppositely charged polyelectrolytes onto porous calcium carbonate (CaCO) particles, followed by core removal. The highly rough surface and the inner cavities of CaCO particles result in a heavy matrix capsule, which can achieve a high solvent encapsulation efficiency and form a micron-sized carrier for the solvent in water that is stable for long times ( at least one week.) Two distinct diffusion coefficients are evidenced by PFG-NMR, which may indicate two distinct diffusion environments in the sample. This suggests that the toluene undergoes a partial exchange between environments within the 100 ms time frame of the NMR experiment.