Organophosphates are prevalent in agrochemicals and chemical warfare agents, posing significant health and safety concerns. These compounds are known for their high chemical stability and to address this issue, nucleophilic catalysts have emerged as a promising solution for their degradation. Herein, we focus on a novel material created through the combined effects of imidazole and crumpled graphene (CG) to develop a nanocatalyst for the neutralization (i.e., degradation) of organophosphates (OPs). The strategy involves the covalent functionalization of CG with imidazole groups without disrupting the three-dimensional structure of CG. This unique combination results in a synergistic effect between neighboring imidazole groups within CG, significantly enhancing the catalytic performance. The catalytic increment (kCAT/kH2O) achieved is in the order of 104 , demonstrating the remarkable efficiency of this catalyst. The pioneering and promising use of functionalized CG for addressing concerns with chemical security can boost and be broadened to other applications.