Graphyne nanoscrolls (GNSs) have attracted significant research interest because of their wide‐ranging applications. However, the production of GNSs via a self‐scrolling approach is environment dependent. Here, molecular dynamics simulations are conducted to evaluate the self‐scrolling behavior of an α‐graphyne (α‐GY) ribbon on a carbon nanotube (CNT) within various multiphysical environments, accounting for the interactions among temperature, electric field, and argon gas. The results demonstrate that the fabrication of an α‐GNS lies in the interplay of van der Waals (vdW) forces among the components in a vacuum. Notably, the α‐GY ribbon is easier to scroll onto a thicker CNT. The electric field attenuates the vdW interaction, necessitating thicker CNTs for successful self‐scrolling under a stronger electric field. In argon, both the vdW interaction and nanoscale pore contribute to the overlap formation. At 300 K, increasing argon density prolongs the time required for α‐GNS formation, with self‐scrolling failing beyond a critical gas density threshold. Moreover, the self‐scrolling becomes easier at higher temperatures. In multiphysical environments, the interplay between the electric field and the gas density dictates the self‐scrolling at low temperatures. Finally, reasonable suggestions are given for successful self‐scrolling. The conclusions offer valuable insights for the practical fabrication of α‐GNS.