Innovation implies successful introduction. Measures of psychophysiological and neural activity have been introduced to political science but the fact they are still rarely used, particularly in mainstream political science, indicates that this introduction has not been successful. Instead, the status quo in political science is to rely on self-reported measures of feelings, beliefs, and opinions. A recent review of research on ``emotion and politics'' in the Annual Review of Political Science underlines this point as it contains very few references to work using measures of psychophysiological and neural activity. We identify three problems with this status quo. First, unconscious (or preconscious) affective processes cannot be measured with self-reports because we are mostly unaware of these processes. Second, the complex interplay between affective and cognitive processes at the neural level cannot be characterized by relying on typical (survey) experimental outcome measures. Third, on socially sensitive topics, people may be motivated to self-report in socially desirable ways. As such, self-reports may even be misleading. In sum, political psychology largely concentrates on more conscious reflections at the expense of potentially relevant preconscious or unconscious explanations or mechanisms. The goal of this chapter is to inspire the next generation of political psychology research to move beyond self-reports and adopt theories and methods that help us to better characterize the affective-cognitive processes of political decision-making. To this end we provide an overview of work using psychophysiological measures (skin conductance, heart rate variability, and facial electromyography (fEMG)), eye-tracking, and neuroimaging measures (electroencephalography (EEG), functional and structural magnetic resonance imaging).