Waste recycling with increasing the lifecycle of resource is a novel approach for enhancing circular economy. Within this context, this study aims to give a second life cycle to phosphogypsum (PG) waste, which is a byproduct from phosphoric acid manufacture, as useful resources. This study evaluates the sustainability of this harmful waste, which is accumulated in large stockpiles and becomes hazardous during storage, and to stabilize bentonite-based concrete intended for road construction. The effect of raw bentonite (Ca-Na montmorillonite), PG, and lime on the properties of cementitious materials has been investigated through various tests. The properties examined include chemistry (X-ray Fluorescence Spectrometry), mineralogy (X-ray Powder Diffraction and Fourier-Transform Infrared Spectroscopy), calorimetry (Differential Thermal Analysis/Thermogravimetry) and microstructure (Scanning Electron Microscopy) of the mortar based on different mixtures of bentonite, PG and lime. The result show that lime and PG addition involves in the formation of new nanocrystalline phases and the disappearance of certain minerals as portlandite. Calcium silicate hydrate gel appeared in the mixture with 8% of lime, whereas strätlingite was neoformed in the mixture with 8% of lime and 8% of PG. These nanocrystalline phases are responsible for enhancing mechanical strength through the pozzoloanic reaction.