Crystalline graphitic nanopetals (GPs), containing a few layers of graphene that grow roughly perpendicularly to a substrate, have attracted much attention in energy storage and sensing applications because of the unique advantages such as large surface area, ultrasharp and exposed edges, fast electron transfer kinetics, and outstanding mechanical, chemical, and electrochemical properties. GPs can be deposited on various substrates using a wide range of precursors (e.g., solids, liquids, or gases) by a catalyst-free plasma-enhanced chemical vapor deposition (PECVD) process. This review provides insights into the growth mechanisms of GPs and their unique properties, and summarizes the latest development of GP-based functional devices for many applications such as electrochemical energy storage and biosensing. Finally, challenges and perspectives for future work are also discussed in this article to fully exploit the potential of the unique graphene material. This review will encourage the applications of GPs in diverse fields and inspire new studies on the exploration of other unique two-dimensional nanostructures.