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Perceived organizational support (POS) in the relationship between neuroticism and job burnout among firefighters received little attention in China. A sampling of 716 firefighters in China, we drew on perceived organization support theory and the notion of support as a buffer in job burnout, examining moderating effects of POS on the relationship between neuroticism and three components of burnout (emotional exhaustion, depersonalization and reduced personal accomplishment). Also, this study explored the mediating effect of burnout on the relationship between neuroticism and mental health (i.e., anxiety and depression). We found that two components (depersonalization and emotional exhaustion) of burnout have significantly mediated the relationship between neuroticism and anxiety and depression. At the same time, POS reinforced the relationship between neuroticism and depersonalization and emotional exhaustion. Therefore, organizations can take our analysis into account when taking actions to improve firefighters' mental health. The implications of these findings were discussed.