Exploring the coupled coordination and interaction between urban transport superiority degree (UTSD) and urban land use efficiency (ULUE) is the key to promoting efficient land use in cities and coordinated development. This paper adopts the improved UTSD model, super-efficiency slack-based measure–undesirable output model, coupling coordination degree model (CCDM), panel Granger causality test, random forest model, and the mixed geographically and temporally weighted regression model to reveal the spatial and temporal evolution and coupling characteristics of UTSD and ULUE in Gansu from 2005 to 2020 and to validate and explore the interaction mechanism between UTSD and ULUE. The results show that (1), from 2005 to 2020, the average UTSD in Gansu increased from 0.56 to 1.01 and the Belt and Road Initiative accelerated the construction of the transportation network in Gansu. The average ULUE increased from 0.52 to 0.62; the spatial distribution of ULUE was high in the west and north and low in the east and south. (2) From 2005 to 2020, the average CCDM of UTSD and ULUE in Gansu increased from slightly unbalanced (0.37) to slightly balanced (0.52). A spatially high UTSD and high ULUE agglomeration area can be found along the transportation arteries. (3) The UTSD and ULUE were mutually causal, with the degree of transportation arterial influence degree being the strongest driver of ULUE among the components of UTSD (30.41% contribution) and tax revenue being the strongest driver of UTSD among the components of ULUE (15.10% contribution). Overall, the connotation of ULUE puts forward the demand for improving the transportation infrastructure and, at the same time, provides the guarantee for UTSD upgrading, which in turn affects the ULUE. In the future, the Xinan region of Gansu should prioritize planning and construction of a transportation network. The results of this study can provide a scientific basis for the construction of transportation networks and the efficient use of urban land in Gansu and other regions.