Photothermoelectric (PTE) materials are promising candidates for solar energy harvesting and photodetection applications, especially for near-infrared (NIR) wavelengths. Although the processability and tunability of organic materials is highly advantageous, examples of organic PTE materials are comparatively rare and their PTE performance is typically limited by poor photothermal (PT) conversion. Here we report the use of redox-active Sn complexes of tetrathiafulvalene-tetrathiolate (TTFtt) as

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... ransmetalating agents for the synthesis of pre-synthetically redox tuned NiTTFtt materials. Unlike the neutral material NiTTFtt, which exhibits n-type glassy-metallic conductivity, the reduced materials Li1.2Ni0.4[NiTTFtt] and [Li(THF)1.5]1.2Ni0.4[NiTTFtt] (THF = tetrahydrofuran) display physical characteristics more consistent with p-type semi-conductors. The broad spectral absorption and electrically conducting nature of these TTFtt-based materials enable highly efficient NIR-thermal conversion and good PTE performance. Furthermore, in contrast to conventional PTE composites, these NiTTFtt coordination polymers are nota-ble as single-component PTE materials. The pre-synthetically tuned metal-to-insulator transition in these NiTTFtt systems directly modulates to their PT and PTE properties.