In order to tap into the advantages of the properties of carbon nanotubes (CNTs) or carbon nanofibres (CNFs) in composites, the high dispersion of CNTs (or CNFs) and strong interfacial bonding are the key issues which are still challenging. In the current work, a novel approach, consisting of in situ synthesis of CNFs within the Cu powders and mixing Cu ions with the in situ CNF(Ni/Y)-Cu composite powders in a solvent, was developed to highly disperse CNFs in a Cu matrix. The composite, produced by vacuum hot pressing, shows extremely high strength, 3.6 times more than that of the matrix material alone. It is worth mentioning that this method can disperse CNFs at high loading in a metal matrix, inferring good potential for applications, such as electronic packaging materials.