Two-dimensional conjugated metal-organic frameworks (2D c-MOFs) are emerging as unique electrode materials with great potential for electronic applications. However, traditional devices based on c-MOFs often utilize them directly in the powder or nanoparticle form, leading to weak adhesion to the device substrate and resulting in low stability and high noise levels in the final device. In this study, we present a novel approach utilizing thin c-MOFs synthesized via a general MOF nanosheet sacrifice approach, enhancing their aspect ratio and flexibility for high-performance electronic applications. The resultant benzene-based Cu-BHT nanosheets feature a thin thickness (around 5 nm) and a high aspect ratio (>100), affording Cu-BHT exceptional flexibility with a 10-fold decrease in Young’s modulus (0.98 GPa) and hardness (0.09 GPa) compared to bulk Cu-BHT nanoparticles (10.79 and 0.75 GPa, respectively). This heightened flexibility enables the Cu-BHT nanosheets to conform to the channels of the electrodes, ensuring robust adhesion to the electrode substrate and improving device stability. As a proof-of-concept, the chemiresistive nanosensor based on Cu-BHT nanosheets demonstrates an 8.0-fold decrease in the coefficient of variation of the response intensity and a 47.1-fold increase in the signal-to-noise ratio compared to sensors based on bulk Cu-BHT nanoparticles. Combined with the machine learning algorithms, the Cu-BHT nanosensor demonstrates outstanding performance in identifying and discriminating multiple volatile organic compounds at room temperature with an average accuracy of 97.9%, surpassing the thus-far-reported chemiresistive sensors.