GdNi is a rare earth intermetallic material that exhibits very interesting magnetic properties. Spontaneous magnetostriction occurs in GdNi at TC, on the order of 8000ppm strain along the c-axis and only until very recently the mechanism causing this giant magnetostriction was not understood. In order to learn more about the electronic and magnetic structure of GdNi, single crystals are required for anisotropic magnetic property measurements. Single crystal processing is quite challenging for GdNi though since the rare-earth transition-metal composition yields a very reactive intermetallic compound. Many crystal growth methods are pursued in this study including crucible free methods, precipitation growths, and specially developed Bridgman crucibles. A plasma-sprayed Gd2O3 W-backed Bridgman crucible was found to be the best means of GdNi single crystal processing. With a source of high-quality single crystals, many magnetization measurements were collected to reveal the magnetic structure of GdNi. Heat capacity and the magnetocaloric effect are also measured on a single crystal sample. The result is a thorough report on high quality single crystal processing and the magnetic properties of GdNi.