Hypertension and osteoporosis are two major chronic diseases affecting the elderly. A cross-sectional study of 3887 Chinese men (n = 1958) and women (n = 1929) was used to explore the association between angiotensin converting enzyme inhibitor (ACEI) use and bone mineral density (BMD). The participants were aged 65 years and above, and were recruited using a combination of private solicitation and public advertising from community centers, housing estates, and the general community in Hong Kong. Demographic, medical, and lifestyle information was obtained from face to face interviews using standardized questionnaire, and physical examination measurements included anthropometry, tibial, and brachial systolic blood pressures, femoral neck, total hip, and lumbar spine BMD. In multiple regression analyses, after adjusting for age, weight, height, thiazide, beta-blocker, calcium channel blocker, statin, corticosteroid, and calcium supplement use, history of diabetes, heart disease, peripheral vascular disease, cigarette smoking, alcohol intake, and physical activity level, ACEI use was associated with higher femoral neck BMD (+0.015 g/cm2, P = 0.035) in women, and higher femoral neck (+0.015 g/cm2, P = 0.017), total hip (+0.016 g/cm2, P = 0.021), and lumbar spine (+0.043 g/cm2, P < 0.001) BMD in men. Thiazide use was associated with higher BMD at all three sites in general, although associations with BMD increase at the total hip (P = 0.07) and femoral neck (P = 0.09) were weak in men. Calcium channel blocker use was only significantly associated with BMD increase at the lumbar spine (P = 0.03) in women, and beta-blocker use did not have significant associations with BMD at any site. This study suggests that in addition to thiazide diuretics ACEI may have possible benefits in treating not only hypertension but also osteoporosis among older Chinese.