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Directed energy deposition (DED) is an additive manufacturing process wherein an energy source is focused on a substrate on which a feedstock material is simultaneously delivered, thereby forming a small melt pool. Melting, solidification, and subsequent cooling occur at high rates with considerable thermal gradients compared with traditional metallurgical processes. Hence, it is important to examine the effects of cooling rates on the microstructures and properties of the additive manufactured materials. In this study, after performing DED with various energy densities, we investigated the changes in the microstructures and Vickers hardness of cast Al-33 wt.% Cu alloy, which is widely used to estimate the cooling rate during processing by measuring the lamellar spacing of the microstructure after solidification. The effects of the energy density on the cooling rate and resultant mechanical properties are discussed, which suggests a simple way to estimate the cooling rate indirectly. This study corresponds to the basic stage of the current study, and will continue to apply DED in the future.