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The use of immobilized microalgae (MA) in bioremediation of wastewaters, in biocapture of nutrients and heavy metals shows an upward trend during recent years. Main advantages of immobilized cells are facilitation of biomass harvesting and increase the stress-tolerance of the cultures. Successful application of the immobilized MA depends on choice of a carrier which should combine a high affinity to cell surface and retention of MA viability. For MA immobilization we tested polymeric materials on the basis of cross-linked highly branched polyethyleneimine (PEI) which is polycationic due to the presence of primary, secondary and tertiary amino groups. PEI easily attaches to the negatively charged cell surface of bacteria and MA and is currently used as a coating agent for facilitating the adhesion of microorganisms to solid surfaces. The investigated PEI sorbents cross-linked with DEG can rapidly and efficiently immobilize cells of both green MA without impairing their viability. The PEI sorbents cross-linked with DEG are good candidates for wastewater treatment with immobilized MA.