The major issue of raw materials’ depletion, and more specifically, of phosphorous (an important fertilizer) has currently become an emergent aspect due to expected depletion problems needing immediate handling. This was the reason for the implementation of the PhoReSe project that aimed to remove and recover phosphorus from the secondary (biologically treated) effluent of a municipal wastewater (biological) treatment plant (WWTP “AINEIA”, located near Thessaloniki, N. Greece), treating the wastewaters of the nearby touristic area. Regarding the phosphorous supplementary removal and recovery treatment options, two methods were examined, initially at the laboratory scale (batch experiments), i.e., (1) the adsorption of phosphorous, and (2) the chemical precipitation of phosphorus. Both methods were further applied at the pilot scale by initially performing the adsorption of phosphorous onto the AquAsZero commercial sorbent, which is a mixed manganese iron oxy-hydroxide, followed by the chemical precipitation of phosphorous implemented after the desorption process of the previously saturated adsorbent. The final precipitate of this procedure was examined as an alternative/supplementary fertilizer, this way returning phosphorus into the natural cycle. These experiments, as applied successfully in at the pilot scale, set the basis for larger-scale relevant applications for similar WWTP facilities.