Marine debris is recognised globally as a key threatening process to marine life, but efforts to address the issue are hampered by the lack of data for many marine habitats. By developing standardised protocols and providing training in their application, we worked with >300 volunteer divers from 11 underwater research groups to document the scale of the subtidal marine debris problem at 120 sites across >1000 km of the coast of NSW, Australia. Sampling consisted of replicated 25×5 m transects in which all debris was identified, counted, and, where appropriate, removed. Sites ranged from estuarine settings adjacent to major population centres, to offshore islands within marine parks. Estuaries and embayments were consistently found to be the most contaminated habitats. Fishing-related items (and especially monofilament and braided fishing line) were most prevalent at the majority of sites, although food and drink items were important contributors at sites adjacent to population centres. The results identified damaging interactions between marine debris and marine biota at some key locations, highlighting the need for management intervention to ensure habitat sustainability. This study reinforces the important contribution that volunteers can make to assessing conservation issues requiring broad-scale data collection. In this case, citizen scientists delivered data that will inform, and help to prioritise, management approaches at both statewide and local scales. These initial data also provide an important baseline for longer-term, volunteer-based monitoring programs.