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The urban canyon albedo (UCA) quantifies the ability of street canyons to reflect solar radiation back to the sky. The UCA is controlled by the solar reflectance of road and façades and the street geometry. This study investigates the variability of UCA in a typical residential area of London and its impact on outdoor and indoor microclimates. The results are based on radiation measurements in real urban canyons and on a 1:10 physical model and simulations using ENVImet v 4.4.6 and EnergyPlus. Different scenarios with increased solar reflectance of roads and façades were simulated to investigate the impact on UCA and street level microclimate. The results showed that increasing the road reflectance has high absolute and relative impact on UCA in wide canyons. In deeper canyons, the absolute impact of the road reflectance is reduced while the relative impact of the walls' reflectance is increased. Results also showed that increasing surface reflectance in urban canyons has a detrimental impact on outdoor thermal comfort, due to increased interreflections between surfaces leading to higher mean radiant temperatures. Increasing the road reflectance also increases the incident diffuse radiation on adjacent buildings, producing a small increase in indoor operative temperatures. The findings were used to discuss the best design strategies to improve the urban thermal environment by using reflective materials in urban canyons without compromising outdoor thermal comfort or indoor thermal environments. [Display omitted] • High reflectance roads are effective in increasing urban albedo in wide canyons. • Façade reflectivity has more potential to increase urban albedo in deep canyons. • High reflectance materials worsen outdoor thermal comfort in urban canyons. • Reducing the façades reflectivity has a positive impact on outdoor thermal comfort. • High reflectance on roads has a negative impact on indoor operative temperatures. [ABSTRACT FROM AUTHOR]