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 gas-cluster 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-to-valley 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 transmission-electron microscopy (HRTEM) shows the crystallinity of the subsurface of the pre- and post-GCIB surfaces to be consistent, following the 1 × 1016 ions/cm2 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 gallium-oxide 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 near-surface layer (less stoichiometric-oxide presence) with use of a CF4/O2 GCIB process. The same peak analysis indicates that the surface gallium-oxide state is nearly unchanged, except in thickness, with the use of an O2-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.