Copper is used for deep geological disposal canisters of spent nuclear fuels, because of excellent corrosion resistance in an oxygen-free environment. However, sulfide formation during the long-term exposure under deep geological disposal condition can be harmful for the integrity of copper canisters. Sulfur around the canisters can diffuse along grain boundaries of copper, causing grain boundary embrittlement by the formation of copper sulfides at the grain boundaries. The development of copper alloys preventing the formation of copper sulfides along grain boundaries is essential for the longterm safety of copper canisters. In this research, the mechanisms of copper sulfide formation at the grain boundary are identified, and possible alloying elements to prevent the copper sulfide formation are searched through the first principle calculations of solute atom-vacancy binding energy and the molecular dynamics calculation of grain boundary segregation energy. The comparison with the experimental literature results on the mitigation of copper embrittlement confirmed that the theoretically identified mechanisms of copper sulfide formation and the selected alloy elements are valid. Thereafter, binary copper alloys were prepared by using a vacuum arc melting furnace. Sulfur was added during casting of the copper alloys to induce the sulfide formation. The cast alloys were cold-rolled into a plate after homogenization heat treatment. The microstructure and mechanical property of each alloy were investigated after recrystallization in a vacuum tube heat treatment furnace. The copper alloys developed in this study are expected to contribute in increasing the long-term safety of deep geological disposal copper canisters by reducing the embrittlement caused by the sulfide formation.