Objective: To investigate the relationship of plasma albumin and hypersensitive C-reactive protein (Hs-CRP) with 5-year all-cause mortality among Chinese older adults aged 65 and older. Method: Data was collected in 8 longevity areas of the Chinese Longitudinal Healthy Longevity Survey (CLHLS) study conducted by Chinese Center for Disease Control and Prevention and Peking University at baseline survey in 2012 and 2014, the participants enrolled in 2012 was followed-up in 2014 and 2017, the participants enrolled in 2014 was followed-up in 2017 only. Finally, 3 118 older adults aged 65 and older with complete information on albumin, Hs-CRP and body mass index (BMI) were included in this study. Plasma samples of older adults were collected for the detection of albumin and Hs-CRP at baseline survey. Survival status and follow-up time was recorded for all participants. All older adults were divided into 4 groups according to the levels of plasma albumin and Hs-CRP, and Cox proportional hazard models were constructed to assess their influence on the risk of all-cause mortality. Results: Among 3 118 older adults included, the prevalence of hypoalbuminemia was 10.1% (316/3 118), and was 22.8% (711/3 118) for elevated Hs-CRP. During 10 132 person-years of follow-up, 1 212 participants died. Participants with hypoalbuminemia had increased risk of all-cause mortality, with an hazard ratio (HR) and 95% confidential interval (CI) of 1.18 (1.01-1.38), compared to participants with normal plasma albuminemia; participants with elevated Hs-CRP had increased risk of all-cause mortality, with an HR (95%CI) of 1.18 (1.04-1.35), compared to participants with normal plasma Hs-CRP. Participants with normal plasma albumin and elevated Hs-CRP, with hypoalbuminemia and normal Hs-CRP, with hypoalbuminemia and elevated Hs-CRP also had increased risk of all-cause mortality when compared to those with normal plasma albumin and normal Hs-CRP, the HR (95%CI) were 1.16 (1.01-1.34), 1.11 (0.91-1.37) and 1.43 (1.11-1.83), respectively. Conclusion: Hypoalbuminemia and elevated Hs-CRP were responsible for increased risk of 5-year all-cause mortality among Chinese older adults from 8 longevity areas.