In general, most physical properties of wood/polyvinyl chloride (PVC) composites are lower than those of corresponding neat PVC resin because of poor interfacial adhesion between the hydrophilic wood flour and hydrophobic PVC. Therefore, in this study, we treated wood flour with three aminosilanes to improve wood/PVC interfacial adhesion strength, and eco-friendly wood/PVC/nanoclay composites were prepared by melt blending the aminosilane-treated wood flour, a heavy metal free PVC compound, and a type of nanoclay. The effects of treating wood flour with the aminosilanes and adding the nanoclay on the mechanical properties of the composites were investigated. Mechanical properties of the composites were investigated by universal testing machine (UTM), izod impact tester, dynamic mechanical analyzer (DMA), and thermomechanical analyzer (TMA). The tensile properties of the composites with the aminosilane-treated wood flour were considerably higher than those of the composites with neat wood flour. Furthermore, a small amount of the nanoclay improved mechanical properties of the composites. The performance of the wood/PVC composites was considerably improved by using the aminosilane-treated wood flour and the nanoclay.