Abstract: The fabrication of planar junctions in carbon nanomaterials is a promising way to increase the optical sensitivity of optoelectronic nanometer-scale devices in photonic connections, sensors, and photovoltaics. Utilizing a unique lithography approach based on direct femtosecond laser processing, a fast and easy technique for modification of single-walled carbon nanotube (SWCNT) optoelectronic properties through localized two-photon oxidation is developed. It results in a novel approach of quasimetallic to semiconducting nanotube conversion so that metal/semiconductor planar junction is formed via local laser patterning. The fabricated planar junction in the field-effect transistors based on individual SWCNT drastically increases the photoresponse of such devices. The broadband photoresponsivity of the two-photon oxidized structures reaches the value of 2 × 107 A W−1 per single SWCNT at 1 V bias voltage. The SWCNT-based transistors with induced metal/semiconductor planar junction can be applied to detect extremely small light intensities with high spatial resolution in photovoltaics, integrated circuits, and telecommunication applications.