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ABSTRACT The increase in demand for advanced electronic components, especially for the new information technologies, calls for an expansion of the materials portfolio and devices. The integration of freestanding transition metal oxide (TMO) membranes with two‐dimensional van der Waals (2DvdW) materials presents a unique opportunity to explore novel interfacial phenomena, driven by their diverse crystal symmetries, bonding characteristics, and electronic correlations. These interactions can lead to the emergence of moiré periodicities, which fundamentally alter the physical properties of the hybrid systems. The interplay of differing symmetries and structural distortions in TMOs and ultrathin 2DvdW materials complicates the prediction of their collective behavior. The twisting of cubic and hexagonal lattices creates complex moiré patterns, while variations in energy scales and correlation strengths further enhance this complexity. Understanding the evolution of moiré periodicity in relation to symmetry and distortion is crucial but remains a significant experimental and theoretical challenge. This perspective explores the integration of 2D van der Waals layers with twisted transition metal oxide (TMO) membranes. We discuss key challenges for both material classes, emphasizing how symmetry, lattice distortions, and electronic correlations govern their structural and electronic behavior. We also examine limitations of current theoretical approaches and argue for the need to develop better multiscale computational methods to model and design these hybrid systems.