Conventionally, metal materials are produced by subtractive manufacturing followed by melting. However, there has been an increasing interest in additive manufacturing, especially metal 3D printing technology, which is relatively inexpensive because of the absence of complicated processing steps. In this study, we focus on the effect of varying powder size on the synthesis quality, and suggest optimum process conditions for the preparation of AlCrFeNi high-entropy alloy powder. The SEM image of the as-fabricated specimens show countless, fine, as-synthesized powders. Furthermore, we have examined the phase and microstructure before and after 3D printing, and found that there are no noticeable changes in the phase or microstructure. However, it was determined that the larger the powder size, the better the Vickers hardness of the material. This study sheds light on the optimization of process conditions in the metal 3D printing field.