The directed self‐assembly of electronic circuits using functional metallic inks has attracted intensive attention because of its high compatibility with extensive applications ranging from soft printed circuits to wearable devices. However, the typical resolution of conventional self‐assembly technologies is not sufficient for practical applications in the rapidly evolving additively manufactured electronics (AMEs) market. Herein, an ultrahigh‐resolution self‐assembly strategy is reported based on a dual‐surface‐architectonics (DSA) process. Inspired by the Tokay gecko, the approach is to endow submicrometer‐scale surface regions with strong adhesion force toward metallic inks via a series of photoirradiation and chemical polarization treatments. The prepared DSA surface enables the directed self‐assembly of electronic circuits with unprecedented 600 nm resolution, suppresses the coffee‐ring effect, and results in a reliable conductivity of 14.1 ± 0.6 µΩ cm. Furthermore, the DSA process enables the layer‐by‐layer fabrication of fully printed organic thin‐film transistors with a short channel length of 1 µm, which results in a large on–off ratio of 106 and a high field‐effect mobility of 0.5 cm2 V−1 s−1. The dual surface architectonics is developed as an ultrahigh‐resolution directed self‐assembly technology for high‐performance soft electronics. The strong adsorbing and pinning effect enables patterning of metal nanoparticle inks with 600 nm resolution. This technology further allows the fabrication of short‐channel organic thin‐film transistors with a high field‐effect mobility of 0.5 cm2 V−1 s−1 and a large on/off ratio of 106.