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Carbon nanomaterials, especially graphene, are promising due to their abundance and the possibility to exploit them in lightweight, flexible, and wearable electronics enabling paradigms such as the Internet of Things. However, conventional methods to synthesize and integrate graphene into functional materials and flexible devices are either hazardous, time demanding, or excessively energy-consuming. To overcome these issues, here we propose a new concept based on the laser processing of single-layer diazonium-functionalized graphene. This is a safe, inexpensive, and environmentally-friendly method making it a competitive alternative for graphene-device fabrication. Flexible chemiresistors exhibit sensitivity for breath (water vapor and CO2) and ethanol detection up to 1500% higher than laser-reduced graphene oxide devices. We attribute this enhanced sensitivity to an optimal balance between structural defects and electrical conductivity. Flexible electronic circuits demonstrate a superb resilience against scratching and high current stability up to 98% with durability against 180° bending cycles for continuous operation of several weeks. This work can impact biomedical technology and electronics where tunable electrical conductivity, sensitivity, and mechanical stability are of uttermost importance.