Abstract: This invention relates to the synthesis of a new generation of metastable aluminum-titanium (Al—Ti) alloys and the process of making them. The preparation method used is a combination process incorporating the advantages of conventional casting and spray techniques. The process is a low cost process. The aluminum-titanium materials made in this invention contain titanium in both the reacted and unreacted form. The results were confirmed using microstructural and x-ray diffraction studies. The presence of phases clearly indicate the metastable nature of these materials in accordance with the equilibrium phase diagram established for Al—Ti system. The Al—Ti materials can be made in the dimensions suitable for structural applications at ambient and elevated temperatures and as control materials for synthesis of more dilute equilibrium Al—Ti materials using conventional techniques such as casting.