Various programs effectively teach children to cross streets more safely, but all are labor- and cost-intensive. Recent developments in mobile phone technology offer opportunity to deliver virtual reality pedestrian environments to mobile smartphone platforms. Such an environment may offer a cost- and labor-effective strategy to teach children to cross streets safely. This study evaluated usability, feasibility, and validity of a smartphone-based virtual pedestrian environment. A total of 68 adults completed 12 virtual crossings within each of two virtual pedestrian environments, one delivered by smartphone and the other a semi-immersive kiosk virtual environment. Participants completed self-report measures of perceived realism and simulator sickness experienced in each virtual environment, plus self-reported demographic and personality characteristics. All participants followed system instructions and used the smartphone-based virtual environment without difficulty. No significant simulator sickness was reported or observed. Users rated the smartphone virtual environment as highly realistic. Convergent validity was detected, with many aspects of pedestrian behavior in the smartphone-based virtual environment matching behavior in the kiosk virtual environment. Anticipated correlations between personality and kiosk virtual reality pedestrian behavior emerged for the smartphone-based system. A smartphone-based virtual environment can be usable and valid. Future research should develop and evaluate such a training system.