Runoff from building and structure surfaces may contribute to the pollution of urban stormwater and, thereby, to the degradation of the receiving water quality. Various micropollutants have been found in surface runoff from buildings in the urban environment, including metals and organic micropollutants. Effective methods for identification of such pollutants and their sources are the prerequisites for the development of control measures. In this paper, three different methods for the identification of building surface materials acting as sources of metals (Cd, Cr, Cu, Ni, Pb and Zn), nonylphenols and phthalates are presented: (i) screening of the material composition, (ii) laboratory leaching experiments with synthetic rainwater, and (iii) open-air pilot testing of material panels exposed to actual rainfall and runoff. These three methods cover a wide span of experimental aspects, including, e.g., size of material samples, resource demands, and control of influential factors. Nine materials commonly used on building and structure surfaces in the urban environment were tested: metal sheets of zinc, copper, galvanised steel, coated corrugated steel and stainless steel; and, four different roofing membranes of bitumen as well as polyvinyl chloride (PVC). The experimental results indicated that all three methods were meritorious in providing some information contributing to the identification of pollutant sources. The screening of material composition for targeted pollutants is relatively quick and inexpensive, but may fail to identify minor sources of pollutants, or may identify the substances present in the material, but not released in contact with water. Laboratory leaching was generally effective in identifying sources of substances present in surface runoff, but was unsuitable for estimating the magnitude of actual concentrations in building runoff. Open-air pilot studies of material samples (exposed area = 2 m2) were thought to provide the results corresponding well to concentrations in runoff from actual building surfaces, but required relatively large financial and labour resources. Thus, the choice of the method for pollutant identification should be based on study objectives, and some benefits may be achieved using more than one method in an integrated manner; e.g., composition screening and lab or open-air leaching of targeted materials.