This study was aimed at examining the relationships of the personality dimensions of the five-factor model or Big Five with trait anger and with two specific traits of hostility (mistrust and confrontational attitude), and identifying the similarities and differences between trait anger and hostility in the framework of the Big Five. In a sample of 353 male and female adults, the Big Five explained a significant percentage of individual differences in trait anger and hostility after controlling the effects due to the relationship between both constructs and content overlapping across scales. In addition, trait anger was primarily associated with neuroticism, whereas mistrust and confrontational attitude were principally related to low agreeableness. These findings are discussed in the context of the anger-hostility-aggression syndrome and the capability of the Big Five for organizing and clarifying related personality constructs.