Raman spectroscopy uses visible light to acquire vibrational fingerprints of molecules, thus making it a powerful tool for chemical analysis in a wide range of media. Its potential for optical imaging at high resolution is, however, severely limited by the fact that the Raman effect is weak. Here, we report the discovery of a giant Raman scattering effect from encapsulated and aggregated dye molecules inside single-walled carbon nanotubes (SWNTs). Measurements performed on rod-like dyes, such as α-sexithiophene and βcarotene, assembled inside SWNTs as highly polarizable J-aggregates indicate a resonant Raman cross-section (CS) of ~10-21 cm 2 /sr, which is well above the CS required for detecting individual aggregates at the highest optical resolution. Free from fluorescence background and photobleaching, this giant Raman effect allows the realization of a library of functionalized and biocompatible nanoprobe labels for Raman imaging with robust detection using multispectral analysis.