Orderly nucleic acid aggregates (ONAAs) self-assembled on mesoporous silica nanoparticles (MSNs) with positively charged aminopropyl groups (PC) were firstly developed. Interestingly, a novel electrostatic DNA self-assembly could realize hybridization chain reaction (HCR) on the surface of PCMSNs in single cells. Significantly, a non-destructive amplification strategy based on ONAAs-PCMSNs was successfully developed for miRNA detection and in situ imaging by the prominent and agminated fluorescence-bright spots in living cells.