The rapid urbanization and increasing traffic have serious social, economic, and environmental impact on metropolitan areas worldwide. It is of a great importance to understand the complex interplay of road networks and traffic conditions. The authors propose a novel framework to estimate traffic conditions at the metropolitan scale using GPS traces. Their approach begins with an initial estimation of network travel times by solving a convex optimization program based on traffic flow theory. Then, they iteratively refine the estimated network travel times and vehicle traversed paths. Last, the authors perform a bilevel optimization process to estimate traffic conditions on road segments that are not covered by GPS data. The evaluation and comparison of the authors' approach over two state-of-the-art methods show up to 96.57% relative improvements. The authors have further conducted field tests by coupling road networks of San Francisco and Beijing with real-world GIS data, which involve 128,701 nodes, 148,899 road segments, and over 26 million GPS traces.