As flexible wearable sensors and imagers are receiving attention from diverse social sectors, the freely attachable photothermoelectric (PTE) conversion technique should be evaluated to develop a highly usable safety sensor network. Although carbon nanotube (CNT)‐related materials should be effective, the key parameters/structures that maximize PTE conversion have not been clarified, thus hindering optimum device design and practical use. Herein, the flexible, sensitive broadband photodetection operation based on a coupling configuration between the CNT film photo/heat/electron channel and metal electrode is evaluated. Experimental PTE measurements and steady‐state thermal distribution simulations reveal that a series coupling of a p‐type CNT film channel and a highly negative Seebeck coefficient counter metal electrode facilitate superior photodetection performances than those of a parallel coupling configuration. Furthermore, subsequent device designs provide sensitive broadband photodetection from the millimeter‐wave to visible light wavelength regions with a minimum noise equivalent power of 5 pWHz−1/2 in an uncooled nonvacuum condition. Simultaneously, the mechanical flexibility of the proposed photodetector allows for its use in freely attachable sheet imager applications on curvilinear objects, and the nondestructive 3D photomonitoring of a defective intricately bent sample is demonstrated.
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