SiO2 nanoparticles capped with gamma-aminopropyltrimethoxysilane were doped into polyelectrolyte (polyallylamine hydrochloride), PAH, and poly(acrylic acid), PAA) multilayer films via spin-assisted layer-by-layer self-assembly. The resulting as-prepared multilayer films were heated at a proper temperature to generate cross-linked composite films with increased adhesion to substrates. The tribological behavior of the multilayer films was evaluated on a microtribometer. It was found that SiO2-doped composite films had better wear resistance than pure polyelectrolyte multilayers, possibly because doped SiO2 nanoparticles were capable of enhancing load-carrying capacity and had "miniature ball bearings" effect. Moreover, heat-treatment had significant effect on the morphology of the composite films. Namely, heat-treated (SiO2/PAA)(9) film had a larger roughness than the as-prepared one, due to heat-treatment-induced agglomeration of SiO2 nanoparticles and initiation of defects. However, heat-treated (PAH/PAA)(3)/(SiO2/PAA)(3)(PAH/PAA)(3) film had greatly reduced roughness than the as-prepared one, and it showed considerably improved wear resistance as well. This could be closely related to the "sandwich-like" Structure of the composite multilayer film. Namely, the outermost Strata of composite multilayer film were able to eliminate defects associated with the middle strata, allowing nanoparticles therein to maintain strength and robustness while keeping soft and fluid-like exposed surface. And the inner strata were well anchored to substrate and acted as an initial "bed" for SiO2 nanoparticles to be inhabited, resulting in good antiwear ability. (C) 2009 Elsevier Inc. All rights reserved.