Biocrust communities provide a pallet of ecosystem services, such as soil stabilization, altering of hydrological cycles and primary production, and often are the first colonizers of unvegetated surfaces during succession. Therefore, artificially establishing biocrusts can improve soil properties, for example, by stabilizing bare soil surfaces against erosion or by accumulating nutrients. In this study, the establishment of artificial biocrusts was tested for the restoration of potash tailings piles that result from potash fertilizer production and mostly consist of NaCl. A biocrust cover as primary vegetation could decrease the saline seepage waters by trapping rainwaters, thereby reducing the environmental pollution. In a laboratory experiment, we created a salt gradient by mixing the tailings materials with non-saline dune sand. Surface material of the abandoned potash tailings pile Neuhof-Ellers (NE) and material of the Infiltration Hampering Stratum (IHS) were tested, along with a treatment with bone charplus (BCplus) and sodium alginate. A mixture of 50% (w/w) IHS and dune sand was most successful for the establishment of green biocrust microalgae, based on increased biomass and photosynthetic performance. The chlorophyll a content was negatively correlated with the electrical conductivity (EC), and was significantly increased in the BCplus and sodium alginate treatment, while biocrusts failed to establish on pure tailings piles substrates. The limit of the substrates EC for biocrust establishment was 35 mS cm−1. This limit provides a baseline for future studies that should use BCplus and sodium alginate to increase the success of biocrust establishment on potash tailings piles.