The Big Five Inventory-2 (BFI-2) has received wide recognition since its publication because it strikes a good balance between content coverage and brevity. The current study translated the BFI-2 into Chinese, evaluated its psychometric properties in four diverse Chinese samples (college students, adult employees, adults treated for substance use, and adolescents), and compared its factor structure with those obtained from two U.S. samples. Across two studies, the Chinese BFI-2 demonstrated good reliability (Cronbach’s α and test–retest reliability), structural validity, convergent/discriminant validity, and criterion-related validity at the domain level. At lower levels of analyses, some facets and negatively worded items functioned better among participants with higher than those with lower education levels. Implications, limitations, and future directions are discussed.