Background: in 2006, Spain implemented a national smoke-free legislation that prohibited smoking in enclosed public places and workplaces (except in hospitality venues). In 2011, it was extended to all hospitality venues and selected outdoor areas (hospital campuses, educational centers, and playgrounds). The objective of the study is to evaluate changes in exposure to secondhand smoke among the adult non-smoking population before the first law (2004-05) and after the second law (2011-12). Methods: repeated cross-sectional survey (2004-2005 and 2011-2012) of a representative sample of the adult (≥16 years) non-smoking population in Barcelona, Spain. We assess self-reported exposure to secondhand smoke (at home, the workplace, during leisure time, and in public/private transportation vehicles) and salivary cotinine concentration. Results: overall, the self-reported exposure to secondhand smoke fell from 75.7% (95%CI: 72.6 to 78.8) in 2004-05 to 56.7% (95%CI: 53.4 to 60.0) in 2011-12. Self-reported exposure decreased from 32.5% to 27.6% (−15.1%, p<0.05) in the home, from 42.9% to 37.5% (−12.6%, p = 0.11) at work/education venues, from 61.3% to 38.9% (−36.5%, p<0.001) during leisure time, and from 12.3% to 3.7% (−69.9%, p<0.001) in public transportation vehicles. Overall, the geometric mean of the salivary cotinine concentration in adult non-smokers fell by 87.2%, from 0.93 ng/mL at baseline to 0.12 ng/mL after legislation (p<0.001). Conclusions: secondhand smoke exposure among non-smokers, assessed both by self-reported exposure and salivary cotinine concentration, decreased after the implementation of a stepwise, comprehensive smoke-free legislation. There was a high reduction in secondhand smoke exposure during leisure time and no displacement of secondhand smoke exposure at home.