Plastic pollution is considered one of today’s major environmental problems. Current land-based monitoring programs typically rely on beach litter data and seldom include plastic pollution further inland. We initiated a citizen science project known as the Mass Experiment inviting schools throughout The Danish Realm (Denmark, Greenland and the Faeroe Islands) to collect litter samples of and document plastic pollution in 8 different nature types. In total approximately 57,000 students (6–19 years) collected 374,082 plastic items in 94 out of 98 Danish municipalities over three weeks during fall 2019. The Mass Experiment was the first scientific survey of plastic litter to cover an entire country. Here we show how citizen science, conducted by students, can be used to fill important knowledge gaps in plastic pollution research, increase public awareness, establish large scale clean-up activities and subsequently provide information to political decision-makers aiming for a more sustainable future.