This article analyses how religious orientations and ideological preferences have coevolved in Chilean society between 1998 and 2014. On the basis of the premise that people experience religion heterogeneously, we develop four hypotheses that describe possible changes in the association between these two variables. Using data from yearly national probability surveys and multinomial regression models, we obtain two general results. First, we observe a general process of political "dealignment," whereby the proportion of the population, religious and irreligious, that ceases to identify with ideological positions strongly increases. Second, the magnitude of this dealignment is moderated by religious denomination and frequency of church attendance. Irreligious people have ceased to identify with ideological positions at higher rates than Evangelicals and Catholics, whereas frequently attending Catholics have become more reluctant than nonattending Catholics to abandon their traditional right-wing preferences. These results imply that as Catholics have reduced their size in the population, they have also become more politically heterogeneous.