The inkjet printing of metal electrodes on polymer films is a desirable manufacturing process due to its simplicity but is limited by the lack of thermal stability and serious delaminating flaws in various aqueous and organic solutions. Kapton, adopted worldwide due to its superior thermal durability, allows the high-temperature sintering of nanoparticle-based metal inks. By carefully selecting inks (Ag and Au) and Kapton substrates (Kapton HN films with a thickness of 135 μm and a thermal resistance of up to 400 °C) with optimal printing parameters and simplified post-treatments (sintering), outstanding film integrity, thermal stability, and antidelaminating features were obtained in both aqueous and organic solutions without any pretreatment strategy (surface modification). These films were applied in four novel devices: a solid-state ion-selective (IS) nitrate (NO 3 − ) sensor, a single-stranded DNA (ssDNA)-based mercury (Hg 2+ ) aptasensor, a low-cost protein printed circuit board (PCB) sensor, and a long-lasting organic thin-film transistor (OTFT). The IS NO 3 − sensor displayed a linear sensitivity range between 10 −4.5 and 10 −1 M (r 2 = 0.9912), with a limit of detection of 2 ppm for NO 3 − . The Hg 2+ sensor exhibited a linear correlation (r 2 = 0.8806) between the change in the transfer resistance (R CT ) and the increasing concentration of Hg 2+ . The protein PCB sensor provided a label-free method for protein detection. Finally, the OTFT demonstrated stable performance, with mobility values in the linear (μ lin ) and saturation (μ sat ) regimes of 0.0083 ± 0.0026 and 0.0237 ± 0.0079 cm 2 V −1 S −1 , respectively, and a threshold voltage (V th ) of −6.75 ± 3.89 V.