Urban greenspace provides opportunities for outdoor exercise and may increase physical activity, with accompanying health benefits. Areas suitable for walking (walkability) are also associated with increased physical activity, but interactions with greenspace are poorly understood. We investigated associations of walkability and green walkability with physical activity in an urban adult cohort. We used cross-sectional data from Greater London UK Biobank participants (n = 57,726) and assessed walkability along roads and footpaths within 1000 m of their residential addresses. Additionally, we assessed green walkability by integrating trees and low-lying vegetation into the walkability index. Physical activity outcomes included self-reported and accelerometer-measured physical activity and active transport. We assessed associations using log-linear, logistic and linear regression models, adjusted for individual- and area-level confounders. Higher green walkability was associated with favourable International Physical Activity Questionnaire responses and achievement of weekly UK government physical activity guideline recommendations. Participants living in the highest versus lowest quintile of green walkability participated in 2.41 min (95% confidence intervals: 0.22, 4.60) additional minutes of moderate-and-vigorous physical activity per day. Higher walkability and green walkability scores were also associated with choosing active transport modes such as walking and cycling. Our green walkability approach demonstrates the utility in accounting for walkability and greenspace simultaneously to understand the role of the built environment on physical activity.