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Functionally graded materials enable the spatial tailoring of properties through controlling compositions and phases that appear as a function of position within a component. The present study investigates the ability to reduce the coefficient of thermal expansion (CTE) of an aluminum alloy, Al 2219, through additions of Ti-6Al-4V. Thermodynamic simulations were used for phase predictions, and homogenization methods were used for CTE predictions of the bulk CTE of samples spanning compositions between 100 wt% Al 2219 and 70 wt% Al 2219 (balance Ti-6Al-4V) in 10 wt% increments. The samples were fabricated using directed energy deposition (DED) additive manufacturing (AM). Al2Cu and fcc phases were experimentally identified in all samples, and aluminides were shown to form in the samples containing Ti-6Al-4V. Thermomechanical analysis was used to measure the CTE of the samples, which agreed with the predicted CTE values from homogenization methods. The present study demonstrates the ability to tailor the CTEs of samples through compositional modification, thermodynamic calculations, and homogenization methods for property predictions.