The course of pupillary constriction and dilation provides an easy-to-access, inexpensive, and noninvasive readout of brain activity. We propose a new taxonomy of factors affecting the pupil and link these to associated neural underpinnings in an ascending hierarchy. In addition to two well-established low-level factors (light level and focal distance), we suggest two further intermediate-level factors, alerting and orienting, and a higher-level factor, executive functioning. Alerting, orienting, and executive functioning - including their respective underlying neural circuitries - overlap with the three principal attentional networks, making pupil size an integrated readout of distinct states of attention. As a now widespread technique, pupillometry is ready to provide meaningful applications and constitutes a viable part of the psychophysiological toolbox.