The morphological and structural changes of an ablated flexible graphite in air and acetone ablation environments were studied here. From field emission scanning electron microscopy (FESEM) images, vertically aligned graphene nanosheets were found on the surface of ablated target in acetone. Measured ablation depth values for the ablated target in water were generally higher than those for the ablated target in air. X‐ray diffraction (XRD) analysis revealed that the (002) peak position and full width at half maximum (FWHM) of this peak in the ablated flexible graphite in the air increased. The gap between the highest occupied molecular orbitals (HOMO) and the lowest unoccupied molecular orbitals (LUMO), i.e., the band gap of the ablated target, indicating that the energy band gap of the ablated target in two ablation media increased compared to the nonirradiated target. Raman analysis from different points of the surface of the ablated target in both ablation media demonstrated the presence of bulk defects on the ablated target in the air, instead the edge defects were found for the ablated target in acetone. From Raman spectra, there were no single‐layer graphene nanosheets pinned on the surface of the target in acetone.