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Photodetection across the near‐infrared (NIR) to short‐wavelength infrared (SWIR) spectrum is important for many applications. This study explores photodetection using nanocrystalline graphite (NCG) in a suspended, narrow constriction configuration for improved performance. Bowtie constrictions are fabricated in both suspended and substrate‐supported NCG devices, allowing for accurate comparison. It shows that the suspended constriction enhances the bolometric photoresponse and sensor detectivity by several orders of magnitude compared to the substrate‐supported counterparts, attributed to reduced thermalization and electric field concentration. The suspended configuration preserves a spectrally flat photoresponse while reducing operating voltage through a tailored NCG layer thickness. Chromatic aberration‐corrected photocurrent spectroscopy is used to measure the photoresponse from 1100 to 1700 nm, and diffraction‐limited hyperspectral photocurrent imaging is conducted to measure the local photocurrent generation across the device. Bolometric and photo‐thermoelectric currents are restricted to the suspended central constriction due to electric field concentration and thermal decoupling and the direction of the photocurrents within the sensor is revealed. The experimental data is complemented by simulations of the light absorption and the electric field distribution. This work indicates the importance of geometry and thermal decoupling for boosting device performance, offering promising prospects for sensitive and low‐power NCG‐based photodetectors in the NIR‐SWIR range.

Graphene is inherently sensitive to vicinal dielectrics and local charge distributions, a property that can be probed by the position of the Dirac point in graphene field‐effect transistors. Exploiting this as a useful sensing principle requires selectivity; however, graphene itself exhibits no molecule‐specific interaction. Complementarily, metal–organic frameworks can be tailored to selective adsorption of specific molecular species. Here, a selective ethanol sensor is demonstrated by growing a surface‐mounted metal–organic framework (SURMOF) directly onto graphene field‐effect transistors (GFETs). Unprecedented shifts of the Dirac point, as large as 15 V, are observed when the SURMOF/GFET is exposed to ethanol, while a vanishingly small response is observed for isopropanol, methanol, and other constituents of the air, including water. The synthesis and conditioning of the hybrid materials sensor with its functional characteristics are described and a model is proposed to explain the origin, magnitude, and direction of the Dirac point voltage shift. Tailoring multiple SURMOFs to adsorb specific gases on an array of such devices thus generates a versatile, selective, and highly sensitive platform for sensing applications.