A novel, three-dimensional (3D), self-supporting material the crumpled graphene ball was developed using an aerosol capillary approach. The resultant crumpled-graphene-ball architecture showed a self-supporting, 3D network microstructure with plenty of ridges and wrinkles. Due to their unique structural characteristics, the 3D balls exhibited a rapid adsorption rate and superior adsorption capacity toward the copper ion (Cu2+). It was noted that the adsorption capacity for Cu2+ reached about 224.56 mg/g within 2 min. A high adsorption capacity, fast adsorption kinetics, excellent regeneration and reusability characteristics, and the ease of materials processing make these crumpled graphene balls ideal candidates for heavy metal ion decontamination in practical application. (C) 2018 Elsevier Inc. All rights reserved.