Usability has a distinct subjective component, yet surprisingly little is known about its neural basis and relation to the neuroanatomy of aesthetics. To begin closing this gap, we conducted two functional magnetic resonance imaging studies in which participants were shown static webpages (in the first study) and videos of interaction with webpages (in the second study). The webpages were controlled so as to exhibit high and low levels of perceived usability and perceived aesthetics. Our results show unique links between perceived usability and brain areas involved in functions such as emotional processing (left fusiform gyrus, superior frontal gyrus), anticipation of physical interaction (precentral gyrus), task intention (anterior cingulate cortex), and linguistic processing (medial and bilateral superior frontal gyri). We use these findings to discuss the brain correlates of perceived usability and the use of fMRI for usability evaluation and for generating new user experiences.