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Partial laser treatment is introduced to carbon‐based microfibers to generate excellent photon sensing capability without bias. This treatment brings about a Seebeck coefficient distribution along the sample's length, out of which a photovoltage with no external bias is generated and sensed. Using a line‐shaped laser spot, carbon microfiber (CMF), graphene microfiber (GMF), and graphene aerogel fiber (GAF) are investigated for their response to µm‐scale photon irradiation. A higher sensitivity for the incident photon is found for the GAF with no position sensitivity. More Seebeck coefficient variation is also observed for the GAF considering the amount of laser power used for the laser treatment. A weaker Seebeck coefficient spatial variation is observed for the GMF compared with the GAF. However, its photovoltage shows an abrupt magnitude change from the laser‐treated region to the non‐treated one. Despite the low spatial variation of the Seebeck coefficient for the CMF, it features an excellent and accurate position‐sensitive photoresponse with polarization change over a distance of ≈100 µm. Such unique capability prompts novel applications in using partially annealed CMF for sensing the position of optical beams at the microscale.

The temperature coefficient of resistivity (θT) of carbon-based materials is a critical property that directly determines their electrical response upon thermal impulses. It could have metal- (positive) or semiconductor-like (negative) behavior, depending on the combined temperature dependence of electron density and electron scattering. Its distribution in space is very difficult to measure and is rarely studied. Here, for the first time, we report that carbon-based micro/nanoscale structures have a strong non-uniform spatial distribution of θT. This distribution is probed by measuring the transient electro-thermal response of the material under extremely localized step laser heating and scanning, which magnifies the local θT effect in the measured transient voltage evolution. For carbon microfibers (CMFs), after electrical current annealing, θT varies from negative to positive from the sample end to the center with a magnitude change of >130% over <1 mm. This θT sign change is confirmed by directly testing smaller segments from different regions of an annealed CMF. For micro-thick carbon nanotube bundles, θT is found to have a relative change of >125% within a length of ∼2 mm, uncovering strong metallic to semiconductive behavior change in space. Our θT scanning technique can be readily extended to nm-thick samples with μm scanning resolution to explore the distribution of θT and provide a deep insight into the local electron conduction.