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In this work, we developed a novel approach for few-layer graphene by employing Li+/Na+ co-intercalated exfoliation assisted by ultrasound method. The experiments were conducted under the ultrasonic power of 300 W and the frequency of 40 kHz without the participation of any organic solvent. The effect of Li+/Na+ proportion on the exfoliation of graphite was intensively investigated. The structure and morphology of the as-exfoliated graphene nanosheets (UGN) was determined by a series of characterizations. The results showed that the th