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Grain-size characteristics of dune networks in the Tengger Desert of northwestern China were investigated. Grain-size parameters (mean, standard deviation, skew, and kurtosis) were determined on dune surfaces at windward toe, stoss, crest and leeward toe locations. Multiple discriminant analyses were applied to distinguish deposition environments. Results indicated that the aeolian sediment is mainly composed of very fine and fine sand in the dune networks of the Tengger Desert. Sorting improves as grain size becomes finer. However, the relationships between mean grain size, skew, and kurtosis vary in space. There is a negative relationship between skew and sorting; similarly, the relationships between sorting and skew, and skew and kurtosis change in space. The sediment deposition environment includes aeolian sediment and lacustrine sediment. The lacustrine sediment provides the source material for dune windward toe and stoss formation and development, but the aeolian sediment provides the source material for dune crest and leeward toe formation and development. According to the log-probability of grain size distributions, aeolian sediments in dune networks are composed of two distinct saltation populations.