Thermochemical decomposition of organic materials under heat-treatment in the absence of oxygen, known as the pyrolysis process, is often employed to convert micro and nano patterned polymers into carbon structures, which are subsequently used as device components. Pyrolysis is performed at ≥900 °C, which entails substrate materials with a high thermal stability that excludes flexible, polymeric substrates. We use optimized laser radiation to pattern graphitic carbon structures onto commercially available polyimide (Kapton) sheets in the micrometer to millimeter scale by inducing a localized, rapid pyrolysis, for the fabrication of flexible devices. Resulting laser carbon films are electrically conductive and exhibit a high-surface area with a hierarchical porosity distribution along their cross-section. The material is obtained using various combinations of laser parameters and pyrolysis environment (oxygen-containing and inert). Extensive characterization of laser carbon is performed to understand the correlation between the material properties and laser parameters, primarily fluence and power. A photothermal carbonization mechani ... mehrsm based on the plume formation is proposed. Further, laser carbon is used for the fabrication of enzymatic, pH-based urea sensors using two approaches: (i) direct urease enzyme immobilization onto carbon and (ii) electrodeposition of an intermediate chitosan layer prior to urease immobilization. This flexible sensor is tested for quantitative urea detection down to 10−4 M concentrations, while a qualitative, color-indicative test is performed on a folded sensor placed inside a tube to demonstrate its compatibility with catheters. Laser carbon is suitable for a variety of other flexible electronics and sensors, can be conveniently integrated with an external circuitry, heating elements, and with other microfabrication techniques such as fluidic platforms.