Organic 1D nanomaterials based on low-molecular-weight semiconducting compounds possess unique properties that can complement or rival those of carbon nanotubes and inorganic 1D nanostructures for applications in nanoscaled optoelectronic devices.[1] For low-cost applications of 1D nanomaterials, it is necessary to develop suitable assembling processes for forming films of nanostructures with good packing order.[2] Attempts to fabricate aligned organic 1D nanostructures by template-assisted synthesis and field-assisted assembly have been reported. [3,4] However, the template-assisted method requires additional steps to remove the templates, whereas the field-assisted assembly method requires an additional process involving an external electric or magnetic field. Recently, evaporation-induced selfassembly has been demonstrated to be a facile way for preparing aligned organic nanowires on a solid substrate.[5] However, an inherent problem of self-assembly is that solid surfaces are often rough at the nanoscale, thereby leading to uneven distribution of the nanostructures and difficulty in achieving uniform films. To cope with this problem, attempts have been made to assemble nanowire monolayer films on a smooth surface and subsequently transfer them to desired solid substrates.Liquid/liquid interfaces have been shown to offer an important platform for the organization of micrometer-or nanometer-sized objects based on interfacial-ordering effects, such as self-assembly of colloid particles, nanoparticles, and viruses.[6] However, there are few reports on the self-assembly of 1D nanostructures at the liquid/liquid interface. [7] The Langmuir-Blodgett (LB) technique has been reported to be a powerful tool for the alignment of pre-prepared 1D inorganic nanostructures at the air/water interface by applying an external compression force at the interface.[8] Herein, we report a simple one-step process for forming and assembling single-crystal organic nanowires into aligned films at the dichloromethane (DCM)/water (liquid/liquid) interface. During evaporation of DCM (organic solvent), organic nanowires are first formed and then self-assembled into ordered films driven by the compression force arising from the shrinking liquid/liquid interface. Upon complete solvent evaporation, a compact monolayer of wellaligned nanowires is left on the water surface. These films can be transferred directly onto any desired substrate or stacked layer-by-layer to form a multilayer film for device applications. Using this simple and low-cost approach, we have prepared a film of squaraine nanowires and fabricated it into a photodetector that shows excellent photoresponse and stability. The result demonstrates that the present method is potentially a versatile and scalable approach to fabricating devices from organic nanostructures.We used squaraines as an example because they are an important class of organic dyes for photonic applications, such as imaging, nonlinear optics, photovoltaics, biological labeling, and photodynamic therapy.[9] ...