Abstract: Graphene nanoplatelets (GnPs) were evaluated against munitions compounds 2,4,6-trinitrotoluene (TNT) and hexahydro-1,3,5-trinitro-s-triazine (RDX) in aqueous solutions for adsorptive removal performance. Fourier transform infrared and Raman spectroscopy were employed to characterize samples and inform adsorption mechanisms. Adsorption kinetics and isotherm studies were conducted in deionized water and compared with granular activated carbon (GAC). Evaluations were conducted with varying pH levels, ionic strengths, and temperatures and with surface water solutions to assess the impact of environmental factors on performance and further inform adsorption mechanisms. This study demonstrated that GnPs exhibited more rapid adsorption than GAC. Furthermore, TNT was adsorbed with greater capacity by GnPs compared to GAC, while GnPs removed RDX in greater capacity only when results were normalized for surface area. The more planar structure of GnPs may have contributed to performance enhancements relative to GAC. Adsorption was not impacted by variations in pH or ionic strength, indicating stable performance in different environments. Thermodynamic analysis indicated that removal was more favorable at higher temperatures. Furthermore, π-π interactions likely facilitated TNT removal by GnPs, while RDX was removed through physisorption by van der Waals forces. This study advanced understanding of environmental management of munitions compounds, as the adsorptive performance of GnPs for munitions compounds in solutions within a natural environmental matrix were evaluated, and key mechanisms supporting adsorptive removal of these compounds were informed. Overall, this study demonstrated the effectiveness of GnPs in treating water contaminated with TNT or RDX, particularly when rapid adsorption is preferred.