Abstract

Organic thin-film transistor (OTFT)-based biosensors have garnered significant attention in life and health monitoring due to their rapid response, label-free detection, and ease of integration. However, in high ionic strength physiological fluids (e.g., blood, saliva), the charges of target biomolecules are shielded by counterions in the solution, resulting in the electrostatic Debye shielding effect. Herein, a unique concave–convex film composed of a Dy–Cu(OH)2 nanomaterial and a conjugated polymer was developed. The convex regions were used to enhance field penetration, and the concave regions were used to suppress the Debye shielding effect, enabling ultrasensitive dual-mode signal responses to TFF3 at the zeptomolar (zM) level. Besides, the detection reliability enhanced by four machine learning algorithms, offering a potential way toward ultraearly diagnosis of cancer biomarkers.