The ongoing urbanization requires enhanced understanding of the local meteorological and climatological conditions within the urban environment for multiple applications, concerning energy demand, human health, and spatial planning. Identifying areas with harmful meteorological conditions enables citizens and local authorities to take actions to optimize quality of life for urban dwellers. At the moment cities have (in general) limited networks of meteorological monitoring stations. To overcome this lack of observations, the use of non-traditional data sources is rapidly increasing. However, the use of such data sources without enough prior verification has become a controversial topic in the scientific community. This study aims to verify and assess one of the main non-traditional data sources, i.e. smartphones. The goal is to research the potential of smartphones (using the Samsung Galaxy S4 as an example phone model) to correctly sense air temperature, relative humidity, and solar radiation, and to determine to what extent environmental conditions negatively affect their performance. The smartphone readings were evaluated against observations from reference instrumentation at a weather station and a mobile measurement platform. We test the response time of the smartphone thermometer and hygrometer, and the light sensor’s cosine response. In a lab setting, we find that a smartphone can provide reliable temperature information when it is not exposed to direct solar radiation. The smartphone’s hygrometer performs better at low relative humidity levels while it can over-saturate at higher levels. The light sensor records show substantial correlation with global radiation observations, and short response times. Measurements along an urban transect of 10 km show the smartphone’s ability to react to fast changes of temperature in the field, both in time and space. However, a bias correction (dependent on wind speed and radiation) is required to represent the reference temperature. Finally we show that after such a bias correction, a smartphone record can successfully capture spatial variability over a transect as well.