Recently, there has been an increasing interest in silver thin film coated polymer spheres as conductive fillers in isotropic conductive adhesives (ICAs). Such ICAs yield resistivities similar to conventional silver flake based ICAs while requiring only a fraction of the silver content. In this work, effects of the nanostructure of silver thin films on inter-particle contact resistance were investigated. The electrical resistivity of ICAs with similar particle content was shown to decrease with increasing coating thickness. Scanning electron micrographs of ion milled cross-sections revealed that the silver coatings formed continuous metallurgical connections at the contacts between the filler particles after adhesive curing at 150°C. The electrical resistivity decreased for all samples after environmental treatment for 3 weeks at 85°C/85% relative humidity. It was concluded that after the metallurgical connections formed, the bulk resistance of these ICAs were no longer dominated by the contact resistance, but by the geometry and nanostructure of the silver coatings. A figure of merit (FoM) was defined based on the ratio between bulk silver resistivity and the ICA resistivity, and this showed that although the resistivity was lowest in the ICAs containing the most silver, the volume of silver was more effectively used in the ICAs with intermediate silver contents. This was attributed to a size effect due to smaller grains in the thickest coating.