In this study, the impact of varying the thickness of the Al2O3 interlayer dielectric on the electrical characteristics of BaTiO3/III‐nitride transistors is investigated. In the findings, it is revealed that a minimum thickness of 8 nm for the Al2O3 layer is crucial to maintain high device performance and protect against sputtering‐induced damage during BaTiO3 deposition. The fabricated BaTiO3/Al2O3/AlGaN/GaN high electron mobility transistors exhibit exceptional electrical properties, including a maximum current density of 700 mA mm−1, an on‐resistance of 5 Ω mm, an ION/IOFF ratio of 107, a subthreshold slope of 119 mV dec−1, and significantly reduced gate leakage current. The devices with the optimal 8 nm Al2O3 thickness demonstrates excellent agreement between theoretical and experimental values for effective mobility, achieving a value of 1188 cm2 V−1·s at a 2D electron gas density of 1013 cm−2. Furthermore, in the study, it is confirmed that increasing the Al2O3 thickness also improves the quality of interface charge density, as evidenced by the results obtained from capacitance–voltage measurements. In these findings, the critical role of controlling the Al2O3 thickness in optimizing the electrical characteristics and overall performance of BaTiO3/III‐nitride transistors are highlighted.