The efficiency of different surface modifications on alumina nanoparticles on both filler dispersion and the final properties of the resulting adhesive nanocomposites have been investigated. A tetraglycidyldiaminodiphenylmethane (TGDDM) epoxy resin and three sample series of nanocomposites were prepared via in-situ incorporation of alumina nanoparticles into the reactor. The alumina/TGDDM nanocomposites were prepared individually using neat or non-treated alumina nanoparticles and two kinds of silane-grafted alumina nanoparticles, i.e., APS-treated alumina and GPS-treated alumina. The presence of different alumina nanoparticles in the epoxy matrices resulted in different states of nanofiller dispersion as revealed in SEM and AFM micrographs. It was elucidated that the silane treatment on alumina nanoparticles is crucial for the desired dispersion in the epoxy matrix. Besides, the appropriate filler dispersion resulted in improved thermal resistance and high degree of cure, especially for the adhesive nanocomposite containing APS-treated alumina nanoparticles. In adhesion tests, the shear strength was improved in both nanocomposites containing silane-grafted alumina with more pronounced values for the nanocomposite containing APS-treated alumina nanoparticles. The shear strength reached from 6.6 MPa for the neat epoxy adhesive to 10.2 MPa for the adhesive nanocomposite containing 5 wt % APS-treated alumina nanoparticles mainly due to high levels of dispersion of the high modulus alumina nanoparticles and effective interfacial interactions with the epoxy matrix. The adhesive peel strength of alumina/TGDDM nanocomposites showed a similar trend as in shear strength with more pronounced variations. A noticeable increase in the peel strength of the nanocomposites containing silane-grafted alumina nanoparticles appeared to correlate with greater levels of crack deflection and hence dissipation of fracture energy as observed in SEM pictures. [ABSTRACT FROM AUTHOR]