Neighborhood walkability can influence physical activity. We evaluated the validity of Walk Score for assessing neighborhood walkability based on GIS (objective) indicators of neighborhood walkability with addresses from four US metropolitan areas with several street network buffer distances (i.e., 400-, 800-, and 1,600-meters). Address data come from the YMCA-Harvard After School Food and Fitness Project, an obesity prevention intervention involving children aged 5–11 years and their families participating in YMCA-administered, after-school programs located in four geographically diverse metropolitan areas in the US (n = 733). GIS data were used to measure multiple objective indicators of neighborhood walkability. Walk Scores were also obtained for the participant’s residential addresses. Spearman correlations between Walk Scores and the GIS neighborhood walkability indicators were calculated as well as Spearman correlations accounting for spatial autocorrelation. There were many significant moderate correlations between Walk Scores and the GIS neighborhood walkability indicators such as density of retail destinations and intersection density (p < 0.05). The magnitude varied by the GIS indicator of neighborhood walkability. Correlations generally became stronger with a larger spatial scale, and there were some geographic differences. Walk Score is free and publicly available for public health researchers and practitioners. Results from our study suggest that Walk Score® is a valid measure of estimating certain aspects of neighborhood walkability, particularly at the 1600-meter buffer. As such, our study confirms and extends the generalizability of previous findings demonstrating that Walk Score is a valid measure of estimating neighborhood walkability in multiple geographic locations and at multiple spatial scales.