Graphene aerogel (GA) is recognized for its high porosity, rendering it a promising candidate for water treatment applications. However, its reuse potential is hampered due to inherent limitations. To address this, the present study introduces a nitrogen-doped graphene aerogel (NGA) developed by integrating polydopamine soft segments and polyaniline hard segments into the GA matrix. This approach promotes the formation of a cohesive and durable 3D network by bridging reduced graphene oxide (rGO) nanosheets, with the hard segments of polyaniline interposed among rGO layers to mitigate significant restacking, thereby enhancing surface area and adsorption sites. NGA demonstrates remarkable properties including strength (67 kPa), reversible compressibility under 64 % strain, low density (12.26 mg/cm3), and thermal stability (Tdecomposition = 679.6 °C in air), which collectively enhance its adsorption capacity and recyclability. This study further examines the influence of various factors such as pH, adsorbates (dyes and organic solvents), initial concentration, and cycle times on the aerogel’s adsorption efficacy. Additionally, simulation outcomes reveal that NGA’s adsorption kinetics and thermodynamics align more closely with the endothermic pseudo-first-order kinetic model, indicative of predominant physical adsorption mechanisms. Given its superior adsorption capabilities for pollutants, NGA holds significant promise for application in water treatment.