This work prepared eco-friendly biocomposites of polyurethane (PU) and sheath palm residues, using castor oil as a polyol. PU composites filled with natural fibers were prepared at different loading rates: 0 to 20 wt.%. Results indicated that the sheath palm was hydrogen-bonded to PU chains and increased the foams' density. Pore size decreased with an increase in fiber content, from 256 to 116 µm. The fiber's addition improved the ductility of PU foams (compressive modulus from 4.74 to 0.26 MPa) and the foams' crystallinity index (from 5.4 to 15.4%). Compared to pristine PU, the composites showed high hydrophobicity (reaching 123° of contact angle for PU-15%) and thermal stability (Tonset from 96 to 96.3°), and high density (from 41 to 60 kg.m−3), making the developed composites an excellent option for environmental applications, such as oil removal and contaminant adsorption.