Post-editing of machine translation is gaining popularity as a solution to the ever-increasing demands placed on human translators. There has been a great deal of research in this area aimed at determining the feasibility of post-editing, and at predicting post-editing effort based on source text features and machine translation errors. However, considerably less is known about the mental workings of post-editing and post-editors' decision-making or, in particular, the relationship between post-editing effort and different mental processes. This paper investigates these issues by analysing data from a think-aloud study through the lens of eye movements and subjective ratings obtained in a separate task. The results show that mental processes associated with grammar and lexis are significantly associated with cognitive effort in post-editing. This association was not observed for other aspects of the task concerning, for example, discourse or the real-world use of the text. In addition, it was noted that lexical issues are linked to long sequences of thought processes. The paper shows that lexis plays a central role in post-editing, and argues that more emphasis should be placed on this issue in future research and in post-editor training.