The effect of embedding Cu-graphene hybrid powder, namely “graphene nano-sheet Cu” (GNS-Cu) powder, into In-40 vol.% Cu solder alloy on the electrical and mechanical properties of In-Cu solder is investigated. GNS-Cu hybrid powders were prepared by mixing reduced graphene oxide powders and CuSO4·5H2O, followed by reduction of the mixture with hydrazine. Subsequently, In-Cu solders with GNS-Cu powders were prepared using a 2-step process, comprising liquid phase sintering (LPS) of In and Cu powders followed by accumulative roll bonding (ARB). During ARB, the GNS-Cu powders were embedded as distinct layers into In-Cu composite solders. Electrical conductivity of the GNS-Cu embedded solders increased by > 20% as compared to pure In-Cu solders processed through the same combination of LPS–ARB steps. The yield strength of In-Cu solder increased by only 10% with the addition of GNS-Cu powders and thus retained the moderate strength often associated with pure In-Cu composite solders. Moreover, the thermal conductivity of GNS-Cu-embedded solders was estimated theoretically to increase by > 60%. These promising findings suggest that GNS-Cu-embedded In-Cu solders can be suitable for next-generation metallic thermal interface material and package-level interconnect applications.