The large strength-to-weight ratio of titanium makes this element an important structural component in the aerospace industry. The strength and other mechanical properties may be further improved by alloying with aluminum to form aluminides, e.g. Ti3Al and TiAl, but at a large loss in ductility. Exposure of the aluminides to hydrogen can cause profound reduction in mechanical stabilities through hydride formation. This paper focuses on the structures of hydride phases in the Ti3Al/H system as determined by neutron diffraction. Another reason for our interest in the aluminides is their possible role as dopants or catalysts in certain complex hydride reactions. A recent report suggests that Ti-doped alkali metal aluminum hydrides may be potentially novel hydrogen storage materials and while the nature of the dopant or catalyst is not known, a titanium aluminide or hydride may be involved.