(How) do individuals’ underlying value orientations matter for populist voting? Building on the congruency model in social psychology, we theorize that voters holding non-conformist values feel closest to political actors employing a taboo-breaking populist style in the political debate. Moreover, we hypothesize that security and universalism values feed into vote choices between right-wing and left-wing parties. Leveraging structural equation modeling (SEM) and data from the 2017 German Longitudinal Election Study (GLES), we find that non-conformist values predict voting for the populist far-right Alternative for Germany (AfD), but not for the left-wing populist The Left. Further, security and universalism values are associated with a higher probability of voting for not only populist but also mainstream parties. These findings point to the underlying role of basic human values in electoral support for populist parties and political behavior in general.