This dataset included 63,085 occurrence records of alien vascular plants from the field surveys of 4,879 sampling plots being conducted in 2010-2015 in Taiwan. We made sample plots with radius in 20 meters along the road systems covering Taiwan and documented the presence of all plants in the plots. The distance between two adjacent sampling points was about 2.0-2.5 kilometers. We georeferenced the center of each sampling plot by using a GPS receiver and documented the coordinate in decimal degrees of latitude and longitude with accuracy to 0.00001 as well as the altitude with accuracy to 1 meter. We documented the coordinates only when GPS signal was fixed and the error of horizontal positioning was within 5 meters. The altitude of sampling point ranged from -17 to 3,155 meters. There were 72 families with 400 species, 18 subspecies, and 9 varieties of alien plants being documented in this dataset.