The grain size characteristics of aeolian sediments are the combined result of sand sources, regional airflow regimes, dune morphology, etc., and are essential for understanding the formation and evolution of barchan dunes. Based on field investigations and laboratory experimental data, in this paper, we explored differences in the grain size characteristics of the surface sediments of barchan dunes at the southeastern edge of the Taklimakan Desert (TKLM-SE), the western (QB-W) and southern parts of the Qaidam Basin Desert (QB-S), the sand belt connecting the Badain Jaran Desert and the Tengger Desert (BT-B), and their responses to sand sources, dune morphology, and wind regimes. The main results were as follows: (i) The mean grian size distribution patterns of the windward slope toe to the leeward slope toe through the dune crest/ridge varied with different transects of the barchan dunes and different deserts, showing four types including gradually fining (GF), gradually coarsening (GC), coarsening followed by fining (CF), and fining followed by coarsening (FC). The patterns were GF and CF in the TKLM-SE; GF, GC, and FC in the BT-B; GF, GC, and CF in the QB-W; and GF in the QB-S. (ii) The interdune sediments provided the source material for the formation and development of barchan dunes and their grain size varied in different deserts. The interdune sediments were composed of gravel and very fine sand in the TKLM-SE, while they were composed of medium and fine sand in the QB-W, QB-S, and BT-B. (iii) The windward side of the barchans varied with different wind directions, and dune height affected dune surface airflow velocity and direction, changing the pattern of grain size distribution on the dune surface. The wind regime over a ten-day or half-month scale could explain the variance in the grain size distribution patterns better than that on an annual scale. (iv) Grain size characteristics of dune surface sands changed with dune shape due to changes in the surface airflow velocity and direction and the sediment-carrying capacity of the airflow. With an increasing ratio of dune height to dune width, the grain size of the dune crest sands became coarser. These results help advance our understanding of the grain size characteristics of barchan dunes and regional variabilities in their patterns.