In the past 17 years, the larger‐scale production of graphene and graphene family materials has proven difficult and costly, thus slowing wider‐scale commercial applications. The quality of the graphene that is prepared on larger scales has often been poor, demonstrating a need for improved quality controls. Here, current industrial graphene synthetic and analytical methods, as well as recent academic advancements in larger‐scale or sustainable synthesis of graphene, defined here as weights more than 200 mg or films larger than 200 cm2, are compiled and reviewed. There is a specific emphasis on recent research in the use of flash Joule heating as a rapid, efficient, and scalable method to produce graphene and other 2D nanomaterials. Reactor design, synthetic strategies, safety considerations, feedstock selection, Raman spectroscopy, and future outlooks for flash Joule heating syntheses are presented. To conclude, the remaining challenges and opportunities in the larger‐scale synthesis of graphene and a perspective on the broader use of flash Joule heating for larger‐scale 2D materials synthesis are discussed.