Based on the near-surface atmospheric turbulence observation in the National Observation and Research Station of Desert Meteorology, Taklimakan Desert of Xinjiang in July 2016, the characteristics of turbulent transport in the unstable atmospheric surface layer in the hinterland of Taklimakan Desert are investigated. With the methods of eddy covariance, quadrant analysis, and spectra analysis, the dissimilarity between the turbulent transport of heat and momentum under different atmospheric instability is analyzed, and its potential physical mechanism is further explored. The results indicate that, under near-neutral conditions, the turbulent transport of heat and momentum is similar. However, as the atmospheric instability increases, the transport dissimilarity between heat and momentum becomes increasingly significant. Heat is transported more efficiently than momentum, while the turbulent transport of momentum shows a great randomness under the strongly thermal condition. This dissimilarity is closely related to the topology of turbulent coherent structures. Under unstable conditions, the coherent structure is dominated by thermal plume. It can induce synchronous changes in potential temperature and vertical velocity, but is difficult to lead corresponding changes in horizontal velocity. The difference in the physical mechanism of turbulent motion is the main reason for the significant dissimilarity between the turbulent transport of heat and momentum with increasing atmospheric instability.