CuFeO2 and CuAlO2 are attractive candidate materials for solar energy harvesting applications such as photocatalysis and photovoltaics. This work describes the structural, optoelectronic, thermal and electric properties of alloyed CuAlxFe1-xO2 Delafossite material synthesized using solid-state sintering techniques. The alloyed samples of CuAlxFe1-xO2 Delafossite oxide consisted of substitution of Fe for Al ranging from x = 0.01 to x = 0.99. The inclusion of Al in low concentrations affects the crystallization rate during solid-state synthesis, dramatically changing the resultant sample morphologies. The addition of dilute amounts of Al also greatly improves the conductivity of the material to a maximum of 3.18 Scm(-1). The material absorption edge shows strong changes over the alloying range. The more highly conducting samples show a strong photoinduced thermoelectric response to Vis-NIR illumination. (C) 2020 Published by Elsevier B.V.