Large-size graphene samples are successfully prepared by combining ultrosonic assisted liquid phase exfoliation process with oxidation-deoxidation method. Different from previous works, we used an ultrasound-treated expanded graphite as the raw material and prepared the graphene via a facile oxidation-reduction reaction. Results of X-ray diffraction and Raman spectroscopy confirm the crystal structure of the as-prepared graphene. Scanning electron microscopy images show that this kind of graphene has a large size (with a diameter over 100 μm), larger than the graphene from graphite powder and flake graphite prepared through single oxidation-deoxidation method. Transmission electron microscopy results also reveal the thin layers of the prepared graphene (number of layers ≤3). Furthermore, the importance of preprocessing the raw materials is also proven. Therefore, this method is an attractive way for preparing graphene with large size.