The association between depression and neuroticism is complex, but due to the difficulty in assessing neuroticism during mood episodes, the mechanisms underlying this relationship remain poorly understood. In this study, we sought to decompose neuroticism into finer-grained elements that were uncorrelated with psychiatric symptoms and to examine the incremental validity of those elements in explaining deficits in interpersonal functioning. A bifactor model with one general factor and six specific factors fit the data well in both a depressed (=807) and a community (=1,284) sample, and the specific factors were relatively independent of acute symptoms. Moreover, two specific factors (Angry Hostility and Self-Consciousness) accounted for incremental variance in interpersonal functioning problems in the community sample and in a subgroup of depressed participants. The results demonstrate that neuroticism can be decomposed into components that are distinct from symptoms and that are incrementally associated with deficits in interpersonal functioning.