Objectives. We examined associations between health literacy and predictors of smoking cessation among 402 low-socioeconomic status (SES), racially/ethnically diverse smokers. Methods. Data were collected as part of a larger study evaluating smoking health risk messages. We conducted multiple linear regression analyses to examine relations between health literacy and predictors of smoking cessation (i.e., nicotine dependence, smoking outcome expectancies, smoking risk perceptions and knowledge, self-efficacy, intentions to quit or reduce smoking). Results. Lower health literacy was associated with higher nicotine dependence, more positive and less negative smoking outcome expectancies, less knowledge about smoking health risks, and lower risk perceptions. Associations remained significant (P < .05) after controlling for demographics and SES-related factors. Conclusions. These results provide the first evidence that low health literacy may serve as a critical and independent risk factor for poor cessation outcomes among low-socioeconomic status, racially/ethnically diverse smokers. Research is needed to investigate potential mechanisms underlying this relationship.