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Novel fabrication schemes are required to deposit nanoscale materials that contain molecules oriented in the plane of the surface. The breakage of in-plane symmetry allows devices to be fabricated in this plane, enabling molecular electronics to follow this successful paradigm of semiconductor devices. The authors discuss here the fabrication of a unique split-tip optical nanoprobe that can be used to both orient molecules on a surface with a strong, localized electric field and deposit them with nanoscale resolution. Ultraviolet light injected through the probe into the region of aligned molecules causes the deposition. The production of the split-tip probe is significantly different than that of the related near-field scanning optical microscope (NSOM) probe, since the stresses in the metal layer must be held by the metal film–silica interface rather than within the film as it encircles the silica of a NSOM probe. Mounting of the probe to ensure reliable electrical contacts is also described.