This study assesses the associations between health literacy and various health behaviors and social factors among older adults, and whether social factors moderate the other associations. Data from 3,241 participants in the LifeLines Cohort Study were analyzed (mean baseline age = 68.9 years). Data on health literacy, health behaviors (physical activity, fruit and vegetable consumption, smoking, breakfast consumption, alcohol consumption, and body mass index (BMI), and social factors (loneliness, social support, social activities, social contacts, and living situation) were collected in three waves. Logistic regression analyses were used, adjusted for age and gender. Low health literacy was associated with insufficient physical activity, insufficient fruit and vegetable consumption, lack of regular breakfast consumption, obesity (odds ratios (ORs) > 1.31, p-values < .005) and low alcohol use (OR = 0.81, p = .013), but not with smoking. Low health literacy was also associated with greater loneliness, engaging in fewer social activities, and having fewer social contacts (ORs > 1.48, p-values < .005), but not with social support or living situation. Only the association between health literacy and smoking was moderated by social contacts, but this finding needs confirmation in future studies. In conclusion, low health literacy is negatively associated with health behaviors and social factors in older adults, but social factors seldom moderate the associations between health literacy and health behaviors.