In this paper, a simple and green method was developed to fabricate a three-dimensional (3D) graphene-based material with the assistance of caffeic acid (CA). The prepared 3D graphene displayed fast and high sorption for norfloxacin (NOR) and ketoprofen (KP). Their adsorption equilibrium was achieved within 12 h for NOR and KP, which was attributed to their fast diffusion in the porous structure of the 3D graphene. The maximum adsorbed amount of this adsorbent was 220.99 mg/g for NOR and 125.37 mg/g for KP according to the Langmuir model at pH 6.6, 298 K. In the competitive adsorption of six pharmaceuticals, the organic compounds in the form of cations are preferentially adsorbed on the adsorbent. The co-existing organic compounds in the actual wastewater do not seriously inhibit the adsorption of NOR and KP. This study provides the theoretical basis for the facile and low-cost preparation of high-performance 3D graphene adsorbents. The results of this study demonstrate the potential utility of 3D graphene as a very effective adsorbent for pharmaceuticals removal from contaminated water.