Hydrothermal procedures are proven methods to produce β-Ca2SiO4 which is one of the major constituents of portland cement. In this study, two alterations in the hydrothermal procedure were made. The first modification was in the source of silica. For this purpose, rice hull ash (RHA) was chosen as the starting material. The second modification was the partial replacement of Ca+2 by Ba+2. Overall, these two modifications led to significant improvements on the hydrothermal process to produce β-Ca2SiO4.