AbstractComplex Ir oxides provide a promising platform for investigating cooperativity and competition between Mott physics and spin‐orbit coupling in condensed matter physics. These materials have the potential to reveal intriguing phases, such as topological phases and the Kitaev spin liquid state, an exactly solvable S = 1/2 spin model describing Ir4+ ions on a 2D honeycomb lattice. However, experimental confirmation of such phases in iridate films has been hindered by the difficulty of preparing (111)‐oriented samples of the perovskite phase. Herein, by constructing SrIrO3/SrTiO3 superlattices on SrTiO3 (111) substrates, (111)‐oriented perovskite phase SrIrO3 films are achieved with the unprecedentedly large thickness of 6 unit cells. Electrical and magnetic characterizations reveal that these films exhibit anomalous Hall insulating behavior, significant charge fluctuations, and long‐range antiferromagnetic order. Moreover, these properties can be tuned by varying the thickness of the SrIrO₃ layer. These emergent phenomena underscore the complex interactions among spin‐orbit coupling, electron–electron correlations, and crystal structure in (111)‐oriented artificial iridate honeycomb lattices. Further, spin fractionalization and topological quantum spin liquid may be achieved by tuning the spin–orbit coupling and crystal field intensity from interface engineering.
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