Word frequency effect has always been of interest for reading research because of its critical role in exploring mental processing underlying reading behaviors. Access to word frequency information has long been considered an indicator of the beginning of lexical processing and the most sensitive marker for studying when the brain begins to extract semantic information Sereno & Rayner, Brain and Cognition, 42, 78-81, (2000), Trends in Cognitive Sciences, 7, 489-493, (2003). While the word frequency effect has been extensively studied in numerous eye-tracking and traditional EEG research using the RSVP paradigm, there is a lack of corresponding evidence in studies of natural reading. To find the neural correlates of the word frequency effect, we conducted a study of Chinese natural reading using EEG and eye-tracking coregistration to examine the time course of lexical processing. Our results reliably showed that the word frequency effect first appeared in the N200 time window and the bilateral occipitotemporal regions. Additionally, the word frequency effect was reflected in the N400 time window, spreading from the occipital region to the central parietal and frontal regions. Our current study provides the first neural correlates for word-frequency effect in natural Chinese reading so far, shedding new light on understanding lexical processing in natural reading and could serve as an important basis for further reading study when considering neural correlates in a realistic manner.