Highly dispersed graphene nanosheets (GNS) are directly integrated into polyurethane sponge for the very first time. Individual GNS with an average thickness of 5 nm were uniformly encapsulated in polyurethane sponge (PUF). Highly durable, flexible, hydrophilic GNS/PUF demonstrated excellent organic dye absorption properties. For a detailed study, we selected typical water-soluble organic dyes such as methylene blue (MB), ethidium bromide (EtBr), eosin Y (EY). The adsorption behavior follows the Langmuir isotherm model indicating strong monolayer chemisorption. Adsorption capacity (lmol/g) of GNS while using in GNS/PUF is 586.8 (MB), 843.1 (EtBr), and 813.3 (EY). Thermodynamic study on the adsorption with three organic dyes using GNS/PUF revealed that the process was spontaneous and exothermic in nature. Additionally, the rate of adsorption is higher and follow the pseudo-second-order kinetic model. The detailed pH-dependent study showed that cationic dyes' adsorption increases with an increase in pH, and anionic dyes follow the opposite trend. The overall results show that the new adsorbent has highly suitable for practical application. (C) 2020 Elsevier Inc. All rights reserved.