Raman scattering microscopy is a versatile tool for label-free imaging and molecular fingerprint analysis.Here,we provide the first demonstration that the selective collection of scattered signals exceeding the critical angle for total inteal reflection enables surface-confined spontaneous Raman investigations at nanometre resolution.This high-axial selectivity leads to improved signal-to-background ratios,thus making this technique an excellent probe for surface-related molecular specimens.The richness of the spectroscopic information obtained through the supercritical angle Raman (SAR) collection path was proven by comparing its output with that of a parallel far-field collection path.Furthermore,we demonstrated that the proposed SAR technique is a versatile microscopy approach that can be used alone or in combination with amplified Raman modalities such as surface-enhanced resonance Raman scattering.