This study investigates the composition–property relationships in ternary engineered geopolymer composites (EGCs) using a simplex centroid design method to optimize the synergy between ground granulated blast furnace slag (GGBS), fly ash (FA), and metakaolin (MK). Mechanical testing revealed that compressive strength (>85 MPa) peaked at 75% GGBS/25% MK, demonstrating MK’s dominant role in enhancing densification, while flexural strength showed a negative correlation with GGBS content but consistent improvement with MK addition. Strain-hardening behavior was most pronounced in 75% GGBS/25% MK and 83% GGBS/8% FA/8% MK mixtures, with the latter achieving optimal precursor synergy. Fiber dispersion uniformity showed a strong linear correlation (R² = 0.98) with tensile strain capacity, confirming its critical role in strain-hardening performance. Mercury intrusion porosimetry analysis demonstrated that the G83F8M8 mixture exhibited the lowest porosity (<10%) and finest pore size distribution (50–100 nm dominant), directly linking pore refinement to superior mechanical properties.