In parallel to the burgeoning field of soft electronics, soft plasmonics concerns about the design and fabrication of plasmonic structures supported on flexible materials. By using 2D closely packed, one-particle thick plasmonic nanoassemblies (i.e. plasmene nanosheets), this thesis has demonstrated three kinds of soft plasmonic structures including elastomer-supported plasmene nanosheets that built from sphere-like and elongated nanoparticles and flexible substrate-supported Janus plasmene nanosheets. The mechanically manipulated plasmonic property and the potential application of soft plasmonic structures have further been illustrated. The successful design of soft plasmonic structures in this thesis indicates some new insight in designing future plasmonic devices.