Despite well-known risks, millions of Americans smoke cigarettes. Researchers have called for new approaches to smoking cessation messages that persuade smokers to quit their habit. Through a series of five web-based studies, this dissertation examines the relationship between smoking-related self-concepts and determinants of smoking cessation. Two smoking-related self-concepts are considered: the smoker self-concept (SSC) and the abstainer self-concept (ASC). This dissertation answers whether value-expressive messages with ASC or SSC frames have potential to increase smoking cessation intentions, self-efficacy, and attitudes. The first study uses a cross-sectional design to describe the relationship between the smoking-related self-concepts and the determinants of smoking cessation. The second study pilot tests messages with ASC and SSC frames and examines their priming and persuasion effects. The third study explores value priorities among smokers and identifies values with the highest and lowest priority. The fourth and fifth studies pilot test ASC and SSC frame messages with values content to ensure that the messages adequately express their respective values. The final study is a web-based survey experiment with a two frame (SSC x ASC) by two value (high priority vs low priority) design with a no message control group. Results provide evidence that smoking-related self-concepts explain variation in the determinants of smoking cessation above and beyond the effects of other smoking-related individual characteristics. ASC and SSC message frames have potential to prime these constructs. Smokers place the highest priority on the value of self-direction, and the least priority on the value of power. Messages that combine an ASC frame with the high priority value of self-direction increase the determinants of smoking cessation among individuals who have low identification with the SSC, but may have unintended boomerang effects on individuals who identity highly with the SSC. The findings support the role of smoking-related self-concepts as individual difference variables that moderate the effects of smoking cessation messages on the determinants of smoking cessation behaviors. Implications of these findings are discussed and directions for future research are proposed.