We studied a NanoBud structure in a local‐scale using high resolution transmission electron microscopy (HRTEM), scanning tunnelling microscopy (STM) and Raman spectroscopy. The HRTEM images show fullerenes on the outer surface of a single‐walled carbon nanotube (SWCNT) and the bonding between the fullerenes and SWCNT were examined by STM measurement, in which the fullerene attachment was stable against high bias imaging. We were also able to perform Raman measurement on a NanoBud structure. Characteristic features of the individual SWCNT, assigned as (16,11), and fullerenes were observed in the vibrational spectrum. The G band and the radial breathing mode (RBM) of SWCNTs as well as an additional feature at 1460 cm–1 were clearly presented simultaneously, which indicate the NanoBud structure.