Ever since the first digital computer—built on hundreds of vacuum tubes—appeared in 1942, computers have evolved from room-sized machines to hand-held devices and transformed our daily lives. This impressive evolution in computers, the same as other modern technologies, is driven by the understanding of new physics, materials, and technologies. Undoubtedly, the next tech-revolution will depend on these likewise. The Two-dimensional material family is one of the promising candidates for future technology. These materials include diverse material species from metals, semiconductors to superconductors and so on, all with layered structures where each layer is only one to few atoms in thickness. Their structures of saturated in-plane covalent bonds result in the out-of-plane interlayer coupling via weak and directionless van der Waals force. These characteristics allow us to assemble any combination of two-dimensional materials layer-by-layer to create unprecedented heterostructures with atomic precision that can host exciting new physics. In this dissertation, I will present my and my colleague’s efforts to develop new methodologies for large-scale, layer-by-layer assembly of two-dimensional materials. These methods enable us to investigate and design the properties of the assembled films on the atomic scale. Based on our methods, we further demonstrate qubits that are built with two-dimensional materials for quantum computers for the first time. The methodologies and demonstrations here, hopefully, will help to pave the way for two-dimensional materials based technology in the future tech-revolution.