We recorded and preprocessed ZuCo 2.0, a new dataset of simultaneous eye-tracking and electroencephalography during natural reading and during annotation. This corpus contains gaze and brain activity data of 739 English sentences, 349 in a normal reading paradigm and 390 in a task-specific paradigm, in which the 18 participants actively search for a semantic relation type in the given sentences as a linguistic annotation task. This new dataset complements ZuCo 1.0 by providing experiments designed to analyze the differences in cognitive processing between natural reading and annotation. The data is freely available here: https://osf.io/2urht/.