The aim of this study was to determine the interaction of surfactant-modified zeolites (SMZ) and orthophosphate (P)-accumulating bacteria in the process of P removal from wastewater. The SMZ were prepared from the natural zeolite (NZ) of size fractions <0.122 mm and 0.25-0.5 mm. The hexadecyltrimethylammonium (HDTMA) bromide was used to modify the NZ surface from partial monolayer to the bilayer coverage. The surface modification of NZ resulted in the change of zeta potential of particles from negative to positive and great enhancement of the P-adsorption capacity. Only in reactors containing <0.122 mm fraction of partial monolayer coverage of the SMZ, the P was efficiently removed from wastewater by combined adsorption onto the SMZ and bacterial uptake in the biomass. The SMZ with bilayer or patchy bilayer coverage showed the bactericidal effect. To enhance the P removal from wastewater in the aerated biological system, the SMZ can be used, but the special attention should be given to the configuration of sorbed HDTMA molecules and its potential desorption.