Vanadium garnet materials and a method for their preparation. The vanadium garnet material has a trivalent vanadium cation and a composition that falls within a specific prismatic-shaped volume in a quaternary composition diagram of MnO, CaO, V.sub.2 O.sub.3, and SiO.sub.2. The prismatic-shaped volume represents compositions of liquids with which said vanadium garnet is in equilibrium on the liquidus surface and from which the vanadium garnet phase is crystallized. A typical vanadium garnet material has the formula Mn.sub.1.3 Ca.sub.1.7 V.sub.2 Si.sub.3 O.sub.12, as provided in the drawing by point F. The vanadium garnet materials may be used in laser applications.