The propensity of Au ions to self-assemble and undergo rapid reduction into colloids and NPs, however, poses distinct barriers for utilizing conventional gold chemistry for creating structurally-defi ned, organized wire structures and thin fi lms. Patterned Au structures have been produced through chemical derivation of gold colloids surfaces [ 14 ] and/or the substrate employed for surface deposition, [15][16][17] or through the aid of physical templates. [18][19][20][21][22] These approaches exhibit shortcomings, both conceptually as well as technically. Specifi cally, Au NP synthesis and surface derivatization are often multi-step procedures and introduce certain variability in term of product uniformity. In addition, in many cases chemical treatment of NPbased fi lms is further required after surface deposition of the NPs, presenting additional experimental parameters to modify and optimize. Furthermore, on a fundamental basis, the rapid reduction of ionic gold into metal NPs severely restricts the possibility to control the structural features and spatial, long-range organization of the metal assemblies.We present a simple strategy for fabricating extremely long (up to several centimeters), horizontally-aligned, conductive gold micro-wires, produced through deposition of a surfactant monolayer upon gold thiocyanate [Au(SCN) 4 − ] aqueous solution. We have recently demonstrated that Au(SCN) 4 − selfassembles into conductive Au 0 nanostructures through singlestep crystallization/reduction process which do not require addition of reducing agents. [23][24][25] Here we show that a surfactant, octyl-melamine (OM), adopts elongated and aligned micro-wire morphology when isothermally compressed at the air/water interface. Furthermore, the OM assemblies constitute a template for gold deposition through electrostatic attraction between the primary amine residues of the surfactant and soluble Au(SCN) 4 − , accompanied by spontaneous crystallization and reduction of gold by the thiocyanate moieties, without addition of reducing agents. In particular, previous studies have demonstrated that immobilization of the gold complex onto amine-displaying surfaces leads to crystalline organization that is largely promoted through aurophilic interactions among Au I species. Reduction leading to metallic gold formation was found to occur concurrently with the crystallization process, overall resulting in surface-anchored Au 0 nanostructure "Bottom-up" technologies are based upon the premise that organized systems -from the nano-scale up to the macro-scale -can be assembled spontaneously from basic building blocks in solution. We demonstrate a simple strategy for the generation of extremely long (up to several centimeters), horizontally-aligned gold micro-wires, produced through a surfactant monolayer template deposited from gold thiocyanate [Au(SCN) 4 − ] aqueous solution. Specifi cally, we show that the surfactant, octyl-maleimide (OM), spontaneously forms oriented micro-wires at the air/water interface, which constitute a templat...