The discovery of graphene has spurred vigorous investigation of 2D materials, revealing a wide range of extraordinary properties and functionalities. 2D heterostructural materials have recently been fabricated by assembling isolated planes layer-by-layer in a desired sequence. Unusual properties and novel physical phenomena have been unveiled in such layered heterostructures. For example, Hofstadters butterfly, an intriguing pattern of the energy states of Bloch electrons, was predicted several decades ago to be observable only under unfeasibly strong magnetic fields in conventional materials. But it has been observed recently under current experimental conditions in graphene/BN layered heterostructures, one of the outstanding new kinds of 2D materials. Moreover, another amazing physics phenomenon, Majorana fermions was predicted to exist in heterostructural systems consisting of a superconductor (SC) and a topological insulator (TI) Journal.