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Aims: This study aimed to investigate whether both high and low levels of low-density lipoprotein cholesterol (LDL-C), i.e., hypercholesterolemia and hypocholesterolemia, were associated with diabetes in Chinese adults. Methods: This cross-sectional study included 22,557 Chinese adults. The LDL-C reference interval was determined from a healthy sub-cohort. Associations between hypocholesterolemia or hypercholesterolemia with diabetes were analyzed using binary logistic regression. Results: The LDL-C reference interval was 1.48–3.77 mmol/L (57.23–145.78 mg/dL). Therefore, hypocholesterolemia, normocholesterolemia, and hypercholesterolemia were defined as an LDL-C concentration of <1.48, 1.48–3.77, and >3.77 mmol/L, respectively. Prevalence of diabetes was higher in people with hypocholesterolemia or hypercholesterolemia than that in people with normocholesterolemia. Hypocholesterolemia was associated with an increased multivariable-adjusted risk for diabetes diagnosis (odds ratio, 1.57; 95% confidence interval, 1.18–2.08), and so was hypercholesterolemia (odds ratio, 1.29; 95% confidence interval, 1.10–1.51). The results remained significant after exclusion of those who took lipid-lowering drugs from the analysis. Conclusions: This study demonstrated that both low and high levels of LDL-C were associated with a higher risk of diabetes diagnosis. Patients with either high or low LDL-C may need to be closely monitored for the risk of diabetes .