The ongoing research in the field of two‐dimensional (2D) materials is motivated by the extraordinary properties of representatives like graphene or MoS2, which might have the potential to revolutionize microelectronics and related fields. However, due to its semimetallic characteristics, graphene is not a suitable candidate for application in semiconductor devices. Transition‐metal dichalcogenides like MoS2 might have a sizeable band gap, but exhibit a considerably lower carrier mobility than graphene. Based on previous experimental and theoretical works, 2D phosphorus carbide seems to be a candidate combining a high carrier mobility with a sizeable and robust band gap. Therefore, the study by Eric R. Heller et al. (article no. 1800192) focuses on 2D phosphorus carbide (PC) polymorphs and their stability and electronic properties using density functional theory calculations including molecular dynamics simulations. In doing so, three novel semiconducting PC structures along with three further semimetallic polymorphs have been found, which show interesting electronic properties and have the potential to stimulate further studies in this field.