Semiconductor-on-diamond (SOD) substrates and methods for making such substrates are provided. In one aspect, a method of making an SOD substrate may include depositing a base layer onto a lattice-orienting silicon (Si) substrate such that the base layer lattice is substantially oriented by the Si substrate, depositing a semiconductor layer onto the base layer such that the semiconductor layer lattice is substantially oriented with respect to the base layer lattice, and disposing a layer of diamond onto the semiconductor layer. The base layer may include numerous materials, including, without limitation, aluminum phosphide (AlP), boron arsenide (BAs), gallium nitride (GaN), indium nitride (InN), and combinations thereof. Additionally, the method may further include removing the lattice-orienting Si substrate and the base layer from the semiconductor layer. In one aspect, the Si substrate may be of a single crystal orientation.