The synthesis of highly complex two-dimensional (2D) metal nanoframes remains a great challenge. Synthetic strategies for preparing 2D metal nanoframes are few, and rational and systematic synthetic pathways to more complicated architectures have not yet been reported. Herein, we demonstrate a stepwise synthetic strategy for complex 2D metal nanoframes with a high degree of intricacy; the strategy leads to a variety of shapes, including rings, triangles, hexagons, and tripods with tailorable single or double frames in a single entity. These nanoframes of high homogeneity could be obtained through selective combination of four different chemical toolkits consisting of selective etching and deposition on certain facets, and concentric and/or eccentric regrowth by controlling the mismatches of lattice constants of metals. The resulting nanoframes were highly homogeneous in size and shape and had van der Waals interactions that maximized rim-to-rim contact, allowing them to uniquely self-assemble into large-area superstructures.