Mesoporous silica (SiO2) spheres are well-known for their excellent chromatographic properties such as the relatively high specific surface, large pore volume, uniform particle size, narrow pore size distribution with favorable pore connectivity; whereas the noble metal Ag nanoparticles have unique size/shape dependant surface plasmon resonance with wide ranging applications. Thus, the desire to synchronize both their properties for specific applications has naturally prompted research in the design and synthesis of core-shell type novel nanoAg@mesoSiO(2) nanocomposites, which display potential utility in applications such as photothermal therapy, photocatalysis, molecular sensing, and photovoltaics. In the present work, SiO2 spheres were carefully functionalized with the monomer, N-vinyl pyrrolidone (NVP), which cohesively controls the uniform mass transfer of Ag+ metal ions, thereby enabling its sequential reduction to zerovalent Ag (in the presence of slightly excess NaOH) by electron transfer from nucleophilic attack of the NVP vinyl group by the water molecules even under ambient conditions. Complete metal nanoshell coverage of the silica surface was obtained after multiple Ag deposition cycles, as systematically confirmed from the BET, TEM, optical and FTIR characterization. Our present Ag-coated silica spheres were directly utilized as viable SERS substrates with high sensitivity in contrast with other long chain polymer/surfactant coated silica spheres, owing to the presence of significant number of nano-gaps enhanced SERS 'hotspots', which were methodically analyzed utilizing two example analytes, such as crystal violet (CV) and calendula officinalis (CaF). (C) 2018 Elsevier B.V. All rights reserved.