Large twist angles in twisted bilayer graphene are widely expected to be electronically trivial, with negligible interlayer coupling and no electronic reconstruction, in contrast to the rich moiré-driven band reconstruction and correlated physics that emerge at small twist angles. Here, we show that this paradigm breaks down near a twist angle of 29°, where the system crosses over between quasicrystalline and commensurate order. Atomic-resolution transmission electron microscopy directly reveals the coexistence of near-dodecagonal quasicrystalline symmetry and emerging moiré periodicity, indicating an intermediate, nonperiodic structural regime. Magnetotransport measurements uncover strong interlayer hybridization mediated by Umklapp scattering, manifested by magneto-intersubband oscillations and a highly unconventional Landau-level spectrum. Remarkably, the Landau-level degeneracy evolves from 4- to 12-fold with increasing temperature, a behavior incompatible with two decoupled graphene monolayers. These findings establish large-angle twisted bilayer graphene as a platform where quasiperiodic symmetry fundamentally reshapes low-energy electronic states beyond the conventional moiré framework.

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• Quantum transport
• Twistronics
• Graphene
• Quasicrystals