Herein we reported a simple way to enrich the large-diameter single-walled carbon nanotubes (SWNTs) by using a mixed concentrated H2SO4/HNO3 treatment. The proportion of the SWNTs with diameter larger than 2 nm measured from transmission electron microscopy was only ca. 3% in the original sample prepared by chemical vapor deposition method. It is found that this proportion becomes remarkably increased with treatment time and reached ca. 20% after 96 h of acid treatment.