A comprehensive study was conducted for a gold nanoparticle (AuNP)-polyethylene (PE) composite. Molecular dynamic (MD) simulations were employed to construct the AuNP-PE systems, achieve their constitutive relations, and measure their tensile properties. Specifically, the AuNP-PE interface/phase was studied via the mass density profile, and its effect was evaluated by comparing the composite with a pure PE matrix. These research studies were followed by the study of the fracture mechanisms and the size and volume fraction effects of AuNPs. Efforts were also made to reveal the underlying physics of the MD simulations. In the present work, an AuNP-PE interface and a densified PE interphase were achieved due to the AuNP-PE van der Waals interaction. Such an interface/phase is found to enhance the Young's modulus and yield stress but decrease the fracture strength and strain.