Gas-cluster ion-beam (GCIB) processing of surfaces provides individual atoms within an accelerated gas cluster (~1,500 atoms per cluster), an energy approximately equal to the individual bond energy of the target surface atoms. The gas-cluster beam is thus capable of providing smoothing and etching of the extreme surface of numerous semiconductors, metals, insulators, and magnetic materials. For semiconductor material systems, the gascluster processing effect on the surface and subsurface material is of critical interest for device and circuitry application integrity. In the case of III-V GaSb, chemo-mechanical or touch polishing is the final step in the semiconductor-wafer manufacturing process, often leaving scratches of various depths or damage on the polished surface. In this paper, we report the GCIB etching and smoothing of chemical-mechanical polished GaSb(100) wafers. Using a dual-energy, dual gas-cluster source process, ∼100 nm of material was removed from a GaSb(100) surface. Atomic-force microscopy (AFM) imaging and power spectral-density (PSD) analysis shows significant decrease in the post-GCIB root-mean-square (Rms) roughness and peak-tovalley measurements for the material systems. X-ray rocking-curve analysis has shown a 24-arcsec reduction in the full-width at half-maximum (FWHM) of the (111) x-ray diffraction peak of GaSb. High-resolution transmissionelectron microscopy (HRTEM) shows the crystallinity of the subsurface of the pre-and post-GCIB surfaces to be consistent, following the 1 × 10 16 ions/cm 2 total-fluence processes, with dislocation density for both pre-and post-GCIB cases below the HRTEM resolution limit. X-ray photoelectron spectroscopy (XPS) indicates a strong Ga 3p electron binding-energy intensity for galliumoxide formation on the GaSb surface with the use of an oxygen GCIB process. Analysis of the Ga 3p electron binding-energy peaks in the XPS data in conjunction with HRTEM indicates a higher Ga or GaSb content in the nearsurface layer (less stoichiometric-oxide presence) with use of a CF 4 /O 2 GCIB process. The same peak analysis indicates that the surface gallium-oxide state is nearly unchanged, except in thickness, with the use of an O 2 -GCIB second step. The material results suggest that GCIB provides a viable method of chemo-mechanical polish (CMP) damage removal on group III-V material for further device processing.