Spin‐Polarized Metallic Metal−Organic Framework With High Conductivity and Half‐Metallic Behavior

The establishment of new concepts for next‐generation conductive materials remains both highly desirable and scientifically challenging. Herein, we report a Cu‐based metal–organic framework (MOF), ([Cu(6Hmna)] n ( 1 , 6Hmna = 6‐mercaptonicotinic acid)), featuring metal–sulfur chains that exhibit intrinsic metallic behavior. Compound 1 exhibits a high electrical conductivity of up to 120 S cm−1, indicating a high electrical conductivity for a MOF in its crystalline form. The metallic transport characteristics are confirmed by temperature‐dependent conductivity measurements. In addition, this Cu‐MOF demonstrates highly efficient photoconductivity, with an outstanding photocurrent responsivity reaching 8100 A W −1 under infrared light illumination. Our theoretical DFT calculations predict that compound 1 exhibits an exotic spin‐polarized electronic structure, in which one spin channel is metallic while the other remains semiconducting. This unique electronic configuration is particularly attractive for applications in spintronics and quantum technologies, as well as in optoelectronic and photoelectrochemical devices.