High-density buckypapers were obtained by using well-aligned carbon nanotube arrays. The density of the buckypapers was as high as 1.39 g cm^–3, which is close to the ultimate density of ideal buckypapers. Then we measured the transport and mechanical properties of the buckypapers. Our results demonstrated that its electrical and thermal conductivities could be almost linearly improved by increasing its density. In particular, its superior thermal conductivity is nearly twice that of common metals, which enables it a lightweight and more efficient heat-transfer materials. The Young’s modulus of the buckypapers could reach a magnitude over 2 GPa, which is greatly improved compared with previous reported results. In view of this, our work provided a simple and convenient method to prepare high-density buckypapers with excellent transport and mechanical properties.