Increasing ocean plastic pollution is irreversibly harming ecosystems and human economic activities. We partner with a non-profit organization and use optimization to help clean up oceans from plastic faster. Specifically, we optimize the route of their plastic collection system in the ocean to maximize the quantity of plastic collected over time. We formulate the problem as a longest path problem in a well-structured graph. However, since collection directly impacts future plastic density, the corresponding edge lengths are non-linear polynomials. After analyzing the structural properties of the edge lengths, we propose a search-and-bound method, which leverages a relaxation of the problem solvable via dynamic programming and clustering, to efficiently find high-quality solutions (within 6%-optimal in practice), and develop a tailored branch-and-bound strategy to solve it to provable optimality. On one-year of ocean data, our optimization-based routing approach increases the quantity of plastic collected by over 60% compared with their current routing strategy, hence speeding up the progress towards plastic-free oceans. It also provides a tool to evaluate the impact of system characteristics on the overall efficiency and inform the design of future systems.