Scalable, Universal In Situ Self-Heating Chemical Vapor Deposition Strategy for High-Quality Thick Turbostratic Graphene via Combined Twist–Tilt Configuration Engineering

High-quality, thick turbostratic graphene offers a promising route to robust, reliable applications while retaining monolayer-like properties. However, its preparation remains challenging, particularly in controlling interlayer configurations and maintaining the quality at high thickness. Herein, an in situ self-heating CVD strategy is developed, realizing simultaneous combined control over twist-tilt interlayer configurations in high-quality, thick graphene. A rapid thermal period stabilizes turbostratic twist stacking by suppressing metastable-to-stable transformation into AB-stacking around the lattice's <i>z</i>-axis, yielding a high layer-number-independent turbostratic ratio (∼92%). Localized self-heating suppresses undesirable gas-phase reactions and amorphous carbon formation, while the electrical "hot-spot" effect facilitates selective defect healing. These suppress tilt configurations around the lattice's <i>x</i>/<i>y</i> axes, resulting in high in-plane interlayer alignment. This strategy achieves low defect density (<10¹⁰ cm^-2) at rapid growth rate (>100 layers hour^-1), rarely accessible via conventional CVD. A self-heating CVD strategy demonstrates excellent scalability and universality, and life cycle assessment and technoeconomic analysis reveal its superior environmental sustainability and cost-effectiveness.