New strategies combining sensitive pathogenic bacterial detection and high antimicrobial efficacy are urgently desirable. Here, we report smart triple-functional Au–Ag-stuffed nanopancakes (AAS-NPs) exhibiting (1) controllably oxidative Ag-etching thickness for simultaneously obtaining the best surface-enhanced Raman scattering (SERS) enhancement and high Ag-loading antibacterial drug delivery, (2) expressive Ag+-accelerated releasing capability under neutral phosphate-buffered saline (PBS) (pH ∼ 7.4) stimulus and robust antibacterial effectiveness involving sustainable Ag+ release, and (3) three-in-one features combining specific discrimination, sensitive detection, and inactivation of different pathogenic bacteria. Originally, AAS-NPs were synthesized by particle growth of the selective Ag-etched Au@Ag nanoparticles with K3[Fe(CN)6], followed by the formation of an unstable Prussian blue analogue for specifically binding with bacteria through the cyano group. Using specific bacterial “fingerprints” resulting from the introduction of dual-function 4-mercaptophenylboronic acid (4-MPBA, serving as both the SERS tag and internal standard) and a SERS sandwich nanostructure that was made of bacteria/SERS tags/AAS-NPs, three bacteria (E. coli, S. aureus, and P. aeruginosa) were highly sensitively discriminated and detected, with a limit of detection of 7 CFU mL–1. Meanwhile, AAS-NPs killed 99% of 1 × 105 CFU mL–1 bacteria within 60 min under PBS (pH ∼ 7.4) pretreatment.
