What constitutes a chiasm is a debated area of research and more often neglected within biblical studies. In response to this, Craig Arnold Smith has produced a work that provides new insights into how to determine whether an author intentionally employs a chiasm. Working from Smith’s method, this paper argues that the Lukan temptation in the wilderness narrative is structured as a chiasm. It also demonstrates how the temptation functions to emphasize certain Lukan themes. Furthermore, it demonstrates that the chiasm of Luke 4:1–14a enhances the interpretive significance of the passage by revealing a literary function that has consequences for the reading of the entirety of Luke-Acts. These functions in turn validate the chiasm of Luke 4:1–14a, illustrating the value of Smith’s methodology.