This study explored the feasibility of fabricating a ZrO2-Zr2Cu ceramic-metal (CERMET) fuel through additive manufacturing (AM) followed by melt infiltration. ZrO2 was selected as a surrogate for UO2 owing to its similar properties, and Zr2Cu was selected owing to its low melting point and neutron absorption cross-section to explore the feasibility of forming a uniform distribution of ceramic particles within a metal matrix. The binder jetting (BJ) AM technique was employed to fabricate preforms with precise control over the particle distribution, addressing the challenges associated with particle agglomeration and ensuring preform shape integrity. Subsequently, spontaneous melt infiltration was employed to achieve a dense and homogeneous CERMET structure. This study emphasized the significance of controlling wettability and surface energies for successful melt infiltration, focusing on the interfacial reactions between Zr2Cu and ZrO2. These results indicate that this novel approach can significantly enhance the thermal and irradiation performance of CERMET fuels.