The supplementary material for (1) related geometric, magnetic and electronic information of the different layer configurations and various two-dimensional honeycomb-Kagome monolayers, (2) band structure with HSE method, Wannier charge center, and distribution of Berry curvature, (3) band structures without and with SOC under different effective Hubbard interaction of the bilayer, trilayer, and quadrilayer Ta2N6C3, (4) band structures of the five- and six-layered Ta2N6C3, and (5) band structures without and with SOC of the Ta2N6C3 monolayer under different biaxial strain and effective Hubbard interaction.