Nanoscale MolecularDiamond products (various diamondoid materials), obtained from petrochemical feedstocks, have been investigated as additives for polypropylene and polycarbonate. Three of the homologues of this family (diamantane, triamantane, and the [121]tetramantane isomer) have marginal effects on the thermal and mechanical properties of nonpolar/semicrystalline polypropylene. Mixtures of methylated tetramantane nanofillers also increase the stress-strain behavior of polypropylene composites without significantly impacting their glass transition temperatures. The addition of the selected diamondoids to amorphous/moderately polar polycarbonate increases the polymer tensile modulus significantly with marginal increases in the yield stress. The effects of the selected diamondoids on the thermal stability, crystallinity, and optical properties of polypropylene and polycarbonate are also reported. The results for the mechanical properties show that the selected diamondoids behave as plasticizers in polypropylene, whereas in polycarbonate, they act as antiplasticizers without adversely affecting the optical clarity.