requires only two parameters: the lattice misalignment angle (θ) between the two single-crystalline grains and the alignment angle (φ) of the GB. It is well documented that GBs greatly affect the electronic, [1][2][3][4][5][6] mechanical, [7][8][9], and thermal properties [5,[10][11][12] of a 2D material, and therefore, GB engineering during 2D materials synthesis and processing is critical for applications. The study of TBs in 3D material is of great interest because of the dominance of TBs in 3D materials and their impact on the mechanical, thermal, and electronic properties of the materials. It is also demonstrated that TBs in 2D materials also have a great impact on their properties [4,10,13,14] but, in contrast, withThe ORCID identification number(s) for the author(s) of this article can be found under