Combining 1D metal nanotubes and nanowires into cross-linked 2D and 3D architectures represents an attractive design strategy for creating tailored unsupported catalysts. Such materials complement the functionality and high surface area of the nanoscale building blocks with the stability, continuous conduction pathways, efficient mass transfer, and convenient handling of a free-standing, interconnected, open-porous superstructure. This review summarizes synthetic approaches toward metal nano-networks of varying dimensionality, including the assembly of colloidal 1D nanostructures, the buildup of nanofibrous networks by electrospinning, and direct, template-assisted deposition methods. It is outlined how the nanostructure, porosity, network architecture, and composition of such materials can be tuned by the fabrication conditions and additional processing steps. Finally, it is shown how these synthetic tools can be employed for designing and optimizing self-supported metal nano-networks for application in electrocatalysis and related fields.