Cities are a major source of litter pollution. Determination of the abundance and composition of plastic litter in cities is imperative for effective pollution management, environmental protection, and sustainable urban development. Therefore, here, a multidisciplinary approach to quantify and classify the abundance of litter in urban environments is proposed. In the present study, litter data collection was integrated via the Pirika smartphone application and conducted image analysis based on deep learning. Pirika was launched in May 2018 and, to date, has collected approximately one million images. Visual classification revealed that the most common types of litter were cans, plastic bags, plastic bottles, cigarette butts, cigarette boxes, and sanitary masks, in that order. The top six categories accounted for approximately 80 % of the total, whereas the top three categories accounted for more than 60 % of the total imaged litter. A deep-learning image processing algorithm was developed to automatically identify the top six litter categories. Both precision and recall derived from the model were higher than 75 %, enabling proper litter categorization. The quantity of litter derived from automated image processing was also plotted on a map using location data acquired concurrently with the images by the smartphone application. Conclusively, this study demonstrates that citizen science supported by smartphone applications and deep learning-based image processing can enable the visualization, quantification, and characterization of street litter in cities.