The assistances of sodium dodecyl benzene sulfonate (SDBS) and aging treatment were introduced to further improve the room-temperature mechanochemical synthesis of the quantum-sized zinc sulfide (ZnS) nanocrystals. As a result, a green strategy for synthesizing the monodisperse nanocrystals with tunable size and crystallinity was developed, holding convenient, highly efficient and low pollution. Size evolution shows a gradually increasing trend along the aging-temperature. A model that the independent reaction cells constructed by SDBS-wrapped reactant packages (solid state vesicles, SSVs) for the confined growth of ZnS nanocrystals was proposed to access the formation mechanism of ZnS quantized crystal in a solid-state synthesis system. The band gaps and band-edge luminescent emissions of as-prepared ZnS nanocrystals experienced the size-dependent quantum confinement effect, while the trap-state emissions exhibited the lattice integrity-dependence. Furthermore, ZnS quantum-sized nanocrystals with narrower size distribution can be obtained by a batch-sorting process through adjusting the centrifugal speed.