© 2020 Elsevier B.V. Silver chain-like nanobelts (NBs) have been prepared by a redox-active ionic liquid (RAIL)|water (W) interfacial method with utilizing the soft interface as a template. A highly hydrophobic RAIL (ferrocenylmethyl)dodecyldimethylammonium tetrakis[3,5-bis(trifluoromethyl)phenyl]borate ([FcMDDA+][TFPB−]) works as both the reducing agent and the liquid substrate in the RAIL|W interfacial system. The morphology of Ag chain-like NBs, which possesses flat surfaces, sharp corners on the edges, and large aspect ratio, combines the features of one-dimensional (1D) and 2D nanostructures. The formation of Ag chain-like NBs is realized by the linkage of small nanounits through an oriented growth along the RAIL|W interface. The size and shape of the Ag deposited at the RAIL|W interface can be controlled by regulating the concentration of Ag precursor in W, where higher (lower) concentration of AgNO3 induces the formation of Ag NBs with smaller (larger) size. The prepared Ag chain-like NBs show good surface enhanced-Raman scattering activity which can be used as the substrate for plasmonic applications.