ABSTRACT:The Raman enhancing ability of noble metal nanoparticles (NPs) is an important factor for surface enhanced Raman scattering (SERS) substrate screening, which is generally evaluated by simply mixing as-prepared NPs with Raman reporters for Raman signal measurements. This method usually leads to incredible results because of the NP surface coverage nonuniformity and reporter-induced NP aggregation. Moreover, it cannot realize in situ, continuous SERS characterization. Herein, we proposed a dynamic SERS monitoring strategy for NPs with precisely tuned structures based on a simplified spatially confined NP growth method. Gold nanorod (AuNR) seed NPs were coated with a mesoporous silica (mSiO 2 ) shell. The permeability of mSiO 2 for both reactive species and Raman reporters rendered the silver overcoating reaction and SERS indication of NP growth. Additionally, the mSiO 2 coating ensured monodisperse NP growth in a Raman reporter-rich reaction system. Moreover, "elastic" features of mSiO 2 were observed for the first time, which is crucial for holding the growing NP without breakage. This feature makes the mSiO 2 coating adhere to metal NPs throughout the growing process, providing a stable Raman reporter distribution microenvironment near the NPs and ensuring that the substrate's SERS ability comparison is accurate. Three types of NPs, i.e., core−shell Au@AgNR@mSiO 2 , Au@AuNR@mSiO 2 , and yolk−shell Au@void@AuNR@mSiO 2 NPs, were synthesized via core−shell overgrowth and galvanic replacement methods, showing the versatility of the approach. The living cell SERS labeling ability of Au@AgNR@mSiO 2 -based tags was also demonstrated. This strategy addresses the problems of multiple batch NP preparation, aggregation, and surface adsorption differentiation, which is a breakthrough for the dynamic comparison of SERS ability of metal NPs with precisely tuned structures and optical properties.