Archaea are major contributors to biogeochemical cycles and energy metabolism among soil microorganisms under extremely acidic and high-temperature conditions, however, the biodiversity and ecological function of archaea in biological soil crusts (BSCs) of desert ecosystems are not fully understood. Here, we used Illumina MiSeq sequencing and microbial functional gene array (GeoChip 5.0) to test the following hypotheses: (1) the composition and function related to biogeochemical cycles of the archaeal community would change significantly in the development process of BSCs; and (2) the key factors driving these changes may be soil biogeochemical properties. The results showed that the diversity, abundance, and functional potential of the archaeal community showed their highest levels in 5-year-old BSCs. The dominant phyla were Thaumarchaeota, Euryarchaeota, and an unclassified phylum in the archaeal community during BSC succession. The functional genes of the archaeal community were mainly involved in carbon (C) and nitrogen (N) cycles, and the functions of the three dominant phyla were complementary in these cycles. Moreover, redundancy analysis showed that soil biogeochemical properties were negatively related to the composition and function of the archaeal community during BSC succession, and the soil C:N ratio might be the major limiting factor. These results provided evidences for our hypotheses and revealed that the archaeal community played an important ecological role in the early development stage of BSCs, and might be pioneer species of soil microbial communities during BSC succession.