Nutrient deficiency is the primary obstacle in tailing ecological restoration besides high heavy metal content. Biological soil crusts (BSCs) are known for their C and N fixation capabilities and play a crucial role in soil P cycle. BSCs are widespread in tailings and provide a potential ecological restoration approach. In 2022, we carried out an on-site restoration on a PbZn tailing pond in Yunnan Province, China. BSCs were propagated by natural moss crust fragment inoculation. The induced moss crusts (IMCs) were monitored at 0, 45, 90, and 135 days and compared with natural moss crusts (NMCs). The chlorophyll-a content and abundance of biotic organisms increased over time, reaching a peak at 135 days and surpassing that of NMCs. Moss crusts increased the content of C, N, and P nutrients and enzyme activities in the 0.5 cm surface soil. They also reduced the DTPA-extractable Pb content. Moss crusts significantly increased the content of fulvic/humic and protein-like/polyphenol substances, thereby raising the humic index of soil dissolved organic matter (especially NMCs). Furthermore, moss crusts also raised the abundance of nitrification (AOB and Nsr), denitrification (narG, napA, qnorB, and nosZ), and P-cycling (gcd, appA, phoC, phoA, and phoD) genes, especially IMCs after a 135-day inoculation. NMCs exhibited higher moss abundance measured via eukaryotic photoautotrophs. Moss crusts increased photosynthetic bacteria abundance (e.g., Leptolyngbya and Nostocales) and reduced the dominance of chemoautotrophic bacteria, especially the dark sulfide oxidation bacteria (Betaproteobacteriales). This trend was more pronounced in NMCs. Overall, IMCs can recover the functions of NMCs, and in some cases (e.g., abundance and diversity of biotic community, soil nutrient and N & P cycle genes), even surpass them. Our research provides new insights into the tailing ecological restoration.