Smartphones, with embedded accelerometers, may be a viable method to monitor gait variability in the free-living environment. However, measurements estimated using smartphones must first be compared to known quantities to ensure validity. This study assessed the validity and reliability of smartphone-derived gait measures compared to a gold-standard footswitch system during overground walking. Seventeen adults completed three 8-minute overground walking trials during 3 separate visits. The stride time series was calculated as the time difference between consecutive right heel contact events within the footswitch and smartphone-accelerometry signals. Linear (average stride time, stride time standard deviation, and stride time coefficient of variation) and nonlinear (fractal scaling index, approximate entropy, and sample entropy) measures were calculated for each stride time series. Bland–Altman plots with 95% limits of agreement assessed agreement between systems. Intraclass correlation coefficients assessed reliability across visits. Bland–Altman plots revealed acceptable limits of agreement for all measures. Intraclass correlation coefficients revealed good-to-excellent reliability for both systems, except for fractal scaling index, which was moderate. The smartphone system is a valid method and performs similarly to gold-standard research equipment. These findings suggest the development and implementation of an inexpensive, easy-to-use, and ubiquitous telehealth instrument that may replace traditional laboratory equipment for use in the free-living environment.