Brain-electric correlates of reading have traditionally been studied with word-by-word presentation, a condition that eliminates important aspects of the normal reading process and precludes direct comparisons between neural activity and oculomotor behavior. In the present study, we investigated effects of word predictability on eye movements (EM) and fixation-related brain potentials (FRPs) during natural sentence reading. Electroencephalogram (EEG) and EM (via video-based eye tracking) were recorded simultaneously while subjects read heterogeneous German sentences, moving their eyes freely over the text. FRPs were time-locked to first-pass reading fixations and analyzed according to the cloze probability of the currently fixated word. We replicated robust effects of word predictability on EMs and the N400 component in FRPs. The data were then used to model the relation among fixation duration, gaze duration, and N400 amplitude, and to trace the time course of EEG effects relative to effects in EM behavior. In an extended Methodological Discussion section, we review 4 technical and data-analytical problems that need to be addressed when FRPs are recorded in free-viewing situations (such as reading, visual search, or scene perception) and propose solutions. Results suggest that EEG recordings during normal vision are feasible and useful to consolidate findings from EEG and eye-tracking studies.