High‐quality dielectric films are indispensable for field‐effect electronic devices to provide high electrical performance. However, deposition of high‐quality dielectric films on flexible substrate remains a challenging task, which greatly limits the electrical performance of flexible or organic field‐effect devices. A room‐temperature deep ultraviolet (DUV) irradiation process is proposed for densification of solution‐processed La2O3 films. It is found that room‐temperature DUV‐La2O3 films not only exhibit leakage and dielectric properties that are comparable to those of high‐temperature annealed‐La2O3 films, but also have very smooth and clean surfaces and excellent bending strain tolerance. The fabricated La2O3 films exhibit a wide band gap (5.78 eV), high dielectric constant (12.68), low leakage density (8.8 × 10−7 A cm−2 at 2 MV cm−1), and high breakdown field strength (3.5 MV cm−1). Organic thin‐film transistors (OTFTs) based on high‐quality solution‐processed La2O3 gate dielectrics show a low operation voltage (≤3 V), low gate leakage current (<10−9 A), and high Ion/Ioff ratio (>105). Based on these room‐temperature‐fabricated high‐performance OTFTs, low‐voltage complementary integrated circuits are successfully fabricated, including complementary inverters and NAND gate circuits. The results demonstrate that room‐temperature DUV‐processed La2O3 films are ideal gate dielectric materials for future flexible and low‐power‐consumption electronic devices.