The Laser Engineered Net Shaping (LENS™) system, a type of directed laser manufacturing, has been used to create compositionally graded materials. Using elemental blends, it is possible to quickly vary composition, thus allowing fundamental aspects of phase transformations and microstructural development for particular alloy systems to be explored. In this work, it is shown that the use of elemental blends has been refined, such that bulk homogeneous specimens can be produced. When tested, the mechanical properties are equivalent to conventionally prepared specimens. Additionally, when elemental blends are used in LENS™ process, it is possible to deposit compositionally graded materials. In addition to the increase in design flexibility that such compositionally graded, net shape, unitized structures offer, they also afford the capability to rapidly explore composition-microstructure-property relationships in a variety of alloy systems. This research effort focuses on the titanium alloy system. Several composition gradients based on different classes of alloys (designated a, a+b, and b alloys) have been produced with the LENS™. Once deposited, such composition gradients have been exploited in two ways. Firstly, binary gradients (based on the Ti-xV and Ti-xMo systems) have been heat treated, allowing the relationships between thermal histories and microstructural features (i.e. phase composition and volume fraction) to be explored. Neural networks have been used to aid in the interpretation of strengthening mechanisms in these binary titanium alloy systems. Secondly, digitized steps in composition have been achieved in the Ti-xAl-yV system. Thus, alloy compositions in the neighborhood of Ti-6Al-4V, the most widely used titanium alloy, have been explored. The results of this have allowed for the investigation of composition-microstructure-property relationships in Ti-6-4 based systems.