AbstractGeopolymer materials are synthetized by the activation of an aluminosilicate source with an alkaline solution. Their properties strongly depend on the polycondensation reaction that is influenced by the raw materials used. Thus, this work aims at studying the influence of reactive or unreactive aluminosilicate sources with different layered structures (T-O-T or T-O) on the geopolymer’s working properties. To this end, six formulations with differences in the metakaolin content and in the addition of mica fillers were synthetized. The structure and the particle’s surface charge of the raw materials were identified and then, the consolidated materials were observed with SEM and characterized by compression testing. The results show that the increase in metakaolin content leads to a decrease in the porosity rate of the geopolymer (from 47 to 40%) and therefore to the improvement of its mechanical properties from 31 to 45 MPa. Besides, the addition of mica provides different microstructure, defined by a growth in the pore size, which modifies the mechanical properties. Finally, a connection between the particle’s surface charge and the specific compressive strength is outlined. As an example, a zeta potential corrected by the reactive volume (ζ*) inferior to -20 leads to a decrease in the geopolymer’s mechanical properties.