A material highway for building up crystal lattices and heterojunctions from molecular layers has been developed based on a concept of combinatorial lattice integration. The atomic-scale precision of automated multilane paving of multilayered thin films is in situ monitored by concurrent reflection high-energy electron diffraction. The designed nanolayered structures are rapidly verified by a concurrent x-ray diffractometer which has been developed for the purpose of this technology. This scheme corresponds to the concurrent two-dimensional Merrifield synthesis to form a variety of sequence-controlled layer structures in parallel and should be widely applicable for systematic fabrication and property screening of nanostructured materials and devices.