Access to fresh fruits and vegetables is a concern, particularly among low-income populations. Mobile vending is one strategy to expand produce availability and access to increase consumption. In 2008, New York City launched a mobile vending initiative, Green Carts. We report on the evaluation. Three waves of cross-sectional observational surveys of produce availability, variety, and quality were conducted during the summers of 2008, 2009, and 2011 in a stratified random sample of stores and carts comparing establishments in Green Cart neighborhoods (n = 13) with comparison neighborhoods (n = 3). Bivariate analyses for availability, variety, and quality comparing Green Cart and comparison neighborhoods were presented across years, and logistic and negative binomial regressions were used to test whether fruit and vegetable availability, variety, and quality increased in Green Cart compared with comparison neighborhoods, adjusting for clustering and neighborhood demographics. Establishments selling fruits and vegetables in Green Cart neighborhoods increased between 2008 and 2011 (50% to 69%, p <0.0001); there was no comparable increase in comparison neighborhoods. Establishments selling more than 10 fruits and vegetables types increased from 31% to 38% (p = 0.0414) in Green Cart neighborhoods; there was no change in comparison neighborhoods. Produce quality was high among comparison establishments, with 95% and 94% meeting the quality threshold in 2008 and 2011, while declining in Green Cart neighborhood establishments from 96% to 88% (p < 0.0001). Sustained produce availability was found in Green Cart neighborhoods between 2008–2011. Green Carts are one strategy contributing to improving produce access among New Yorkers.