Two polyurethane polyaniline nanocomposites have been synthesized using two in situ polymerization routes of dried and wet bases to valorize the polyurethane waste. The physical and chemical properties of polyurethane-based nanocomposites were compared using SEM, XRD, FTIR, and Zeta potential. SEM images showed that the average particle size of the dried-based composite was 56 nm, while the wet-based composite had an average size of 75 nm. The separation efficiency for methylene blue (MB) and Congo red (CR) dyes was evaluated against free polyurethane foam waste. It was evident that pure polyurethane (PPU) achieved only 4.79% and 16.71% removal for MB and CR, respectively. These dye decontamination efficiencies were enhanced after nano polyaniline decoration of polyurethane foam either through dried base polymerization (DPUP) or wet base polymerization (WPUP). WPUP composite records 11.23% and 85.99% for MB and CR removal, respectively, improved to 26.69% and 90.07% removal using DPUP composite for the respective dyes. The adsorption kinetics, isotherms, and thermodynamics were investigated. The experimental results revealed the pseudo-second-order kinetic model as the most accurately described kinetics model for both CR and MB adsorption. The Langmuir model provided the best fit for the data, with maximum adsorption capacities of 110.98 mg/g for CR and 26.86 mg/g for MB, with corresponding R-squared values of 0.9974 and 0.9608, respectively. Regeneration and reusability studies of PPU, WPUP, and DPUP showed effective reusability, with DPUP displaying the highest adsorption capacity. These results aid in creating eco-friendly and cost-efficient adsorbents for dye removal in environmental sanitation.