There is a need for intraoperative imaging technologies to guide breast-conserving surgeries and to reduce the high rates of re-excision for patients in which residual tumor is found at the surgical margins during post-operative pathology analyses. Feasibility studies have shown that utilizing topically applied surface-enhanced Raman scattering (SERS) nanoparticles (NPs), in conjunction with the ratiometric imaging of targeted vs. untargeted NPs, enables the rapid visualization of multiple cell-surface biomarkers of cancer that are over-expressed at the surfaces of freshly excised breast tissues. In order to reliably and rapidly perform multiplexed Raman-encoded molecular imaging (REMI) of large numbers of biomarkers (with 5 or more NP flavors), an enhanced staining method has been developed in which tissue surfaces are cyclically dipped into a NP-staining solution and subjected to high-frequency mechanical vibration. This dipping and mechanical vibration (DMV) method promotes the convection of the SERS NPs at fresh tissues surfaces, which accelerates their binding to their respective biomarker targets. By utilizing a custom-developed device for automated DMV staining, we demonstrate the ability to simultaneously image 4 cell-surface biomarkers of cancer at the surfaces of fresh human breast tissues with a mixture of 5 flavors of SERS NPs (4 targeted and 1 untargeted control) topically applied for 5 min and imaged at a spatial resolution of 0.5 mm and a raster-scanned imaging rate of >5 cm2/min.