Objective: Smoking is a major cause of worldwide morbidity and mortality. Evidence-based intervention programs to help young adults quit smoking are largely lacking; identifying targets for intervention is therefore critical. A candidate target is inhibitory control, with previous studies on Go/No-Go trainings showing behavior change in the food and alcohol domain. The current study examined the mechanisms of change of HitnRun, a Go/No-Go game, in a smoking population that was motivated to quit. Methods: A two-armed experimental study (n = 106) was conducted and young adults (Mage = 22.15; SDage = 2.59) were randomly assigned to either play HitnRun or to read a psychoeducational brochure. Prior to and directly following the intervention period, smoking-specific and general inhibitory control, perceived attractiveness of smoking pictures, and weekly smoking behavior were assessed. Results: Results indicate that Go/No-Go training seems to be effective in decreasing evaluations of smoking stimuli rather than top-down smoking-specific and general control processes. Similar reductions for weekly smoking were found in both groups. Conclusions: We conclude that HitnRun shows some promise, but more research and iterative design is needed to create a multi-component intervention for smoking cessation that is dynamically adjustable to the individual needs of young people.