[Objective] The coupling relationships of land use efficiency between urban and rural areas were explored in order to provide decision support for sustainable, endogenous and high-quality development of the region. [Methods] By building a three-stage DEA (data envelopment analysis) model to measure and evaluate the urban-rural land use efficiency of 69 counties (cities and districts) in Zhejiang Province from 2006 to 2018, and using the coupling coordination model, the paper explored the coordination level of urban and rural land use efficiency and their spatio-temporal evolution characteristics. [Results] ① The urban-rural land use efficiency was obviously different across Zhejiang Province, and the scale level was the main influencing factor of land use efficiency; ② The urban land use efficiency among counties (cities and districts) was not significantly different, while the spatial polarization of agricultural land use efficiency was significant. ③ From 2006 to 2018, the coupling and coordination degree of urban-rural land use efficiency in Zhejiang Province showed a fluctuating ascending trend, depending on the level of agricultural land use efficiency. ④ There are obvious regional differences in the coordination degree between urban-rural land use efficiency. [Conclusion] The urban-rural land use efficiency in Zhejiang Province is greatly affected by the external environment, and improving agricultural land use efficiency is the key to realize urban-rural coordination and high-quality development.