https://doi.org/10.1002/adma.201805665 Computational modeling and simulations play an integral role in the bottom‐up design and characterization of graph‐n‐yne materials. Here, the state of the art in modeling α‐, β‐, γ‐, δ‐, and 6,6,12‐graphyne nanosheets for synthesizing graph‐2‐yne materials and 3D architectures thereof is discussed. Different synthesis methods are described and a broad overview of computational characterizations of graph‐n‐yne's electrical, chemical, and thermal properties is provided. Furthermore, a series of in‐depth computational studies that delve into the specifics of graph‐n‐yne's mechanical strength and porosity, which confer superior performance for separation and desalination membranes, are reviewed.