The adhesive joint between silica nanoparticles and ultrathin poly(vinylpyridine) (PVP) layers (thickness between 3 and 100 nm) was tested using the cantilever of an atomic force microscope. Specifically, the strength of the adhesive bond (or practical adhesion) was probed in a tearing contact mode, when the particle was removed by applying a tangential force parallel to the substrate surface. The effect of the polymer molecular weight and layer thickness on the particle (practical) adhesion was investigated. It was found that the particles were removed by destroying the cohesive contact zone and that the PVP layer thickness had a pronounced effect on the force needed to destroy the adhesive joint. In particular, the greater the layer thickness, the larger was the required break force. However, the strength of the adhesive joint was estimated to be higher for a thinner layer. It is suggested that mechanical properties of the system as well as molecular characteristics of the PVP layer are responsible for the trend observed. The molecular weight of the polymer did not significantly affect the strength of the adhesive bond.