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We developed polyurethane foams (PU) filled with eucalyptus charcoal residue (ECR) (5, 10, 20, and 30% by wt) for diesel sorption from seawater. The PU foams were characterized by FTIR, FT-Raman, SEM, density, TGA, contact angle, diesel S500 and S10 sorption, and recyclability. The ECR addition altered PU chemical structure, inducing new chemical bonds and probably altering cross-linking ability of the foams, as indicated by FTIR. FT-Raman spectra of PU-ECR foams showed shifts associated with filler dispersion and interaction with the matrix; besides, its addition decreased the foam pore size and density. The ECR addition did not significantly change the thermal behavior of PU foam and increased hydrophilicity in low ECR content and hydrophobicity in high ECR content samples. Experimental results showed adequate oil sorption capacity, and the optimal amount was 30% (by wt) ECR, which enhanced the diesel sorption from 4.1 and 5.9 g.g−1 to 9.6 and 8.8 g.g−1 for diesel S500 and S10, respectively. The Langmuir sorption isotherm was the best-fitting model to describe oil sorption. Reusability of the PU + 30% ECR was examined through 34 and 39 cycles for diesel S500 and S10, and about 50% of the initial sorption capacity remained at the end. The results indicated the success of developing a sustainable material and demonstrating feasibility in practical applications of PU-ECR foam for spilled oil removal from seawater or treatment of oily effluents.