Two fumed silicas, one hydrophilic and another hydrophobic, were added to a two-component polyurethane (PU) adhesive and their properties compared. The filled polyurethanes were characterized by thermal gravimetric analysis (TGA), differential scanning calorimetry (DSC), transmission electron microscopy (TEM), and water and diiodomethane contact angle measurements. The adhesive strength was evaluated from single lap-shear tests of solvent wiped stainless steel/polyurethane adhesive joints. The fumed silicas were well-dispersed in the polyurethane matrix as bundles of nanometric spherical silica particles. However, some micron size agglomerates of fumed silica appeared in the filled polyurethane. The addition of fumed silica favoured the degree of phase separation between the hard and the soft segments in the polyurethane. The polyurethanes were not fully cured under the conditions used in this study and the addition of fumed silica inhibited the curing reaction; the extent of the curing reaction was not affected by the hydrophilic or hydrophobic nature of the fumed silica. The filled polyurethanes were further cured during DSC experiments and this was noticed by the appearance of the melting of the hard segments and the displacement of the second glass transition to a higher temperature. On the other hand, the addition of fumed silica increased the wettability and the surface energy of the polyurethane; this increase was mainly due to an increase in the polar component of the surface energy. The increase in surface energy is somewhat more marked in the case of the hydrophilic silica filled polyurethane, indicating that the polarity of the fumed silica affected the surface properties of the polyurethane. Finally, the addition of the hydrophilic fumed silica increased the adhesion of the filled polyurethane adhesive to stainless steel which was in agreement with the higher surface energy of the hydrophilic fumed silica filled polyurethane. (C) Koninklijke Brill NV, Leiden, 2012