Experiments with multi-walled carbon nanotubes (MWCNTs) and graphite as targets in a source of negative ions with cesium sputtering (SNICS) have shown that MWCNTs with nm radii and μm length can be compared with μm-size graphite grains to understand the irradiation effects that include the formation, sputtering of carbon clusters and the resulting structural changes. The simultaneous adsorption of Cs˚ on the surface and bombardment by energetic Cs + is shown to play its role in the cluster formation and sputtering of carbon atoms and clusters (C x ; x ≥1) and the cesium-substituted carbon clusters (CsC x ) as anions. Sputtered species' qualitative and quantitative outputs are related to their respective structures. Structural changes are shown to occur in MWCNTs and seen in SEM micrographs. The individual identity of the heavily bombarded MWCNTs may have given way to the merged structures while effects on the structure of heavily irradiated graphite grains size needs to be further investigated.