An appropriate wavelength of light impinging on a noble metal nanostructure can cause the conduction-band electrons to oscillate collectively, resulting in localized surface plasmon resonance (LSPR) excitation. [1,2] This process generates enhanced electromagnetic (EM) fields at the surface of the nanostructure that can be several orders of magnitude larger than the incident optical excitation fields, [2][3][4][5][6] leading to many types of surface-enhanced phenomena, [3,5,[7][8][9][10][11][12][13][14] including surface-enhanced Raman scattering (SERS). SERS has been extensively studied for several decades, [5,15] and it is often described as a near-field phenomenon that occurs when the Raman-active molecules are in proximity to the surface of the nanostructure, as the enhanced EM fields decay rapidly with distance from its surface. [15][16][17] The decay lengths have been reported to be in the range of a few nanometers and depend on the size, shape, and composition of the nanostructure. [18,19] Recently, we developed a process termed on-wire lithography (OWL) [20] for the construction of nanostructures from one-dimensional wires by using a template synthesis method. [21][22][23][24] OWL allows rod and disk structures to be made with sub-5 nm to many micrometers feature size. Importantly, it allows generation of nanostructures over different compositions adjacent to one another. Therefore, OWL allows important distance-dependent phenomena in many areas to be probed, [25,26] including molecular electronics, catalysis, spectroscopy, and optics. Indeed, it is an excellent test bed for probing some of the fundamental underpinnings of the SERS phenomenon.Herein, we describe how OWL can be used to fabricate nanostructures made of gold that have excitable plasmon resonances in the visible region of the spectrum (632.8 nm), and which are separated by nanometer-scale distances from nickel segments that do not have such plasmon resonances but can be selectively modified with Raman-active probes. We have discovered that disklike gold nanostructures can be separated from the nickel segments by 120 nm and can still exhibit enhanced Raman scattering using the Raman probes, although the probes are only localized on the nickel segment. This is an unprecedented example of long-range SERS. This long-range surface enhancement constitutes a method for using plasmon excitation to enhance photoprocesses over distances that are relevant to applications in chemical and biological sensing.In a typical experiment, OWL is used to fabricate a 360 nm diameter multisegmented nanowire containing: 1) a 1.5 mm segment of gold, 2) a 1.5 mm gap, 3) a pair of (120 AE 18) nm long gold nanodisks that are separated by a (30 AE 10) nm gap (termed a gold nanodisk pair), and 4) a 1.5 mm nickel wire segment that is separated by a (120 AE 13) nm gap from the gold nanodisk pair (Figure 1 a, left to right). The 120 nm gold disk thickness and 30 nm gap distance were chosen based upon previous results from our group that show a near-ideal geometry for obtaini...