Smoking is a major cause of worldwide morbidity and mortality. There is no evidence-based intervention program available to help young adults quit smoking; identifying targets for intervention is critical. A candidate target is inhibitory control, with previous studies showing behavior change in the food and alcohol domain by applying Go/No-Go training paradigms. The current study examined the mechanisms of change of HitnRun, a video game based on principles of Go/No-Go training, in a smoking population that was motivated to quit. A two-armed randomized controlled trial (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 revealed no improvements in smoking-specific inhibitory control in either intervention group. Similar improvements for general inhibitory control and weekly smoking behavior were observed for both groups. However, the game intervention group showed larger improvements for evaluations of untrained smoking stimuli compared to the brochure intervention group. Results indicate that Go/No-Go training seems to be effective in training devaluation of motivational smoking stimuli rather than top-down control processes. Therefore, we conclude that HitnRun shows some promise, but more research and iterative design is needed to invest in creating a multi-component intervention for smoking cessation that is dynamically adjustable to individual needs to reach as many young people as possible.