This study aims to test the pathways of change from individual exposure to smoke-free legislation on smoking cessation, as hypothesized in the International Tobacco Control (ITC) Conceptual Model. A nationally representative sample of Dutch smokers aged 15 years and older was surveyed during 4 consecutive annual surveys. Of the 1,820 baseline smokers, 1,012 participated in the fourth survey. Structural Equation Modeling was employed to test a model of the effects of individual exposure to smoke-free legislation through policy-specific variables (support for smoke-free legislation and awareness of the harm of [secondhand] smoking) and psychosocial mediators (attitudes, subjective norm, self-efficacy, and intention to quit) on quit attempts and quit success. The effect of individual exposure to smoke-free legislation on smoking cessation was mediated by 1 pathway via support for smoke-free legislation, attitudes about quitting, and intention to quit smoking. Exposure to smoke-free legislation also influenced awareness of the harm of (secondhand) smoking, which in turn influenced the subjective norm about quitting. However, only attitudes about quitting were significantly associated with intention to quit smoking, whereas subjective norm and self-efficacy for quitting were not. Intention to quit predicted quit attempts and quit success, and self-efficacy for quitting predicted quit success. Our findings support the ITC Conceptual Model, which hypothesized that policies influence smoking cessation through policy-specific variables and psychosocial mediators. Smoke-free legislation may increase smoking cessation, provided that it succeeds in influencing support for the legislation.