Located at the collision boundary between the Philippine Sea Plate and the Eurasian Continental Plate, the island of Taiwan is generally recognized as an important example in the MARGINS Program Science Plan and "source-to-sink" research because of its high tectonic activity, heavy rainfall and unique geography. Large suspended sediment loads are transported to the adjacent ocean by Taiwanese rivers every year, making Taiwan an important source of sediments into the adjacent seas and a natural laboratory for studying the systemic movement of fluvial sediments from source to sink. A detailed study on the clay mineral composition of surface sediments collected from the drainage basins of 12 Taiwanese rivers using X-ray diffraction methods was conducted. Our results indicated that the clay mineral assemblages consisted dominantly of illite (approximately 73%) and chlorite (approximately 24%), with lesser abundances of kaolinite (approximately 3%) and even lower levels of smectite from the Danshuei River sediments in northwestern Taiwan. The Jhuoshuei River sediments from western Taiwan contained clay mineral assemblages that consisted of illite (approximately 75%) and chlorite (approximately 25%), but they lacked kaolinite and smectite. In southwestern Taiwan, the clay mineral assemblages were dominated by illite (approximately 75%) and chlorite (approximately 23%), but had a low abundance of kaolinite (generally < 2%) and no smectite. The clay mineral assemblages in eastern Taiwan are obviously different from those in western parts of the island. The most noticeable difference is that the average abundance of chlorite in the Hualien River from eastern Taiwan was the highest (approximately 48%) of all the Taiwanese rivers. We concluded that, in general, the clay mineral assemblages in Taiwanese rivers were mainly composed of illite and chlorite with kaolinite and smectite being scarce, and these trends are different from those in China's mainland rivers. The clay mineral composition shown in this study was primarily determined by the properties of the bedrock, and the differential weathering intensities of the drainage area. The surface sediments in Taiwan's rivers showed a greater abundance of illite and chlorite because the outcropped rocks were mainly composed of Tertiary sedimentary rocks, especially sandstone, shale and slate, and show strong physical weathering. The relatively high relief and more abundant rainfall also caused the clay minerals in the fluvial sediments to be transported to the estuaries down rivers from the mountains and then delivered to the adjacent seas by currents and waves over a shorter time scale.