Dementia cases are on the rise and researchers seek innovative ways to prevent or ameliorate cognitive impairment in later life. Some research has reported that combining mental and physical exercise may benefit cognition more than either alone. This randomized pilot trial examined the feasibility and cognitive benefit for older adults (n = 30) of a single bout of neuro-exergaming (physical activity with cognitive training) using an interactive physical and cognitive exercise system (iPACES), compared with that of exergaming or neurogaming alone. Intent-to-treat and sensitivity analyses were conducted using repeated-measures ANOVA, controlling for age, sex, and education. A significant interaction effect was found for executive function (Color Trails 2), with a significant improvement in the neuro-exergaming condition. Results demonstrate feasibility for older adults to use a novel and theoretically-derived neuro-exergame, and also provide promising new evidence that neuro-exergaming can yield greater cognitive benefit than either of its component parts.