We report on co-existing dual anisotropy ripple formation, sp bonding transformation, and variation in the delocalized π electron system in 1 keV Ar+ ion irradiated few-layer graphene surfaces. Ripples in directions, perpendicular and parallel to the ion beam were found. The irradiation effect and the transition from the sp2-bonding to sp3-hybridized state were analyzed from the deconvolution of the C (1s) peak and from the shape of the derivative of the Auger transition spectra. The results suggest a plausible mechanism for tailoring of few-layer graphene electronic band structure with interlayer coupling tuned by the ion irradiation.