Therefore, graphene becomes a rising star on the horizon of materials science. Since the first report of centimeter-scale single-crystal graphene by Ruoff group showed high electrical quality, [9] great achievements have been made in the fabrication of high-quality graphene for the application in electronic devices, including single-crystalline graphene flakes, [10,11] super-ordered graphene structures, [12,13] super-clean graphene films, [14-16] and ultra-flat graphene films. [17] However, the zero-bandgap feature for monolayer graphene has limited its potential applications in semiconductors. In addition, the negligible mass, low yield, and high production costs of graphene are insurmountable bottlenecks for the practical application in energy conversion and storage. In particular, the absence of killer applications leads to the increased difficulty in graphene commercialization. [18,19] Nevertheless, it is undeniable that the unique structure of graphene has sparked intense interest in condensed matter physics, such as fractional quantum Hall effects, [17] proton permeation, [20] and plasmons. [21] More interestingly, twisted bilayer graphene (tBLG), which is similar to the van der Waals heterostructures, has a dramatic effect on the electronic properties. [22,23] The relative rotating graphene layers become a powerful model to study topological physical properties, including ferromagnetism, [24] Mott insulating behavior and superconducting behaviors, [25,26] topological valley transport, [27] van Hove singularities, [28] and tunable bandgap. [29] Consequently, the twisted structure of tBLG has triggered tremendous enthusiasm, even inspiring the formation of a new field for twisted 2D materials. Currently, production methods of tBLG contain chemical vapor deposition (CVD) on metal catalysts; [30] epitaxial growth on SiC substrate; [31] folding monolayer graphene, [32] and stacking monolayer graphene. [33] These methods are divided into two categories: direct growth and manual assembly. Generally, the direct growth of tBLG undergoes an in situ rearrangement of carbon atoms in the non-equilibrium state at high temperatures, whereas the ex situ vertical overlap of monolayer graphene by transfer process is the basic principle for manual assembly. The completely different preparation processes give rise to the distinctive advantages and disadvantages, but precise control over twist angle and super-clean interface are the ultimate pursuits for any preparation method. Recent progress in Twisted bilayer graphene (tBLG) exhibits a host of innovative physical phenomena owing to the formation of moiré superlattice. Especially, the discovery of superconducting behavior has generated new interest in graphene. The growing studies of tBLG mainly focus on its physical properties, while the fabrication of high-quality tBLG is a prerequisite for achieving the desired properties due to the great dependence on the twist angle and the interfacial contact. Here, the cutting-edge preparation strategies and challenges of tBLG fabrica...