Pollutants deposited on road surfaces and distributed in the environment are a source of nonpoint pollution. Field data are traditionally hard to collect from roads because of constant traffic. In this study, in cooperation with the traffic administration, the dry deposition on and road runoff from urban roads was measured in Taipei City and New Taipei City, Taiwan. The results showed that the dry deposition is 2.01–5.14 g/m2·day and 78–87% of these solids are in the 75–300 µm size range. The heavy metals in the dry deposited particles are mainly Fe, Zn, and Na, with average concentrations of 34,978, 1,519 and 1,502 ppm, respectively. Elevated express roads show the highest heavy metal concentrations. Not only the number of vehicles, but also the speed of the traffic should be considered as factors that influence road pollution, as high speeds may accelerate vehicle wear and deposit more heavy metals on road surfaces. In addition to dry deposition, the runoff and water quality was analyzed every five minutes during the first two hours of storm events to capture the properties of the first flush road runoff. The sample mean concentration (SMC) from three roads demonstrated that the first flush runoff had a high pollution content, notably for suspended solid (SS), chemical oxygen demand (COD), oil and grease, Pb, and Zn. Regular sweeping and onsite water treatment facilities are suggested to minimize the pollution from urban roads.