The use of fluid catalytic cracking (FCC) by-products as aluminosilicate precursors in geopolymer binders has attracted significant interest from researchers in recent years owing to their high alumina and silica contents. Introduced in this study is the use of geopolymer concrete comprising FCC residue combined with fly ash as the requisite source of aluminosilicate. Fly ash was replaced with various FCC residue contents ranging from 0–100% by mass of binder. Results from standard testing methods showed that geopolymer concrete rheological properties such as yield stress and plastic viscosity as well as mechanical properties including compressive strength, flexural strength, and elastic modulus were affected significantly by the FCC residue content. With alkali liquid to geopolymer solid ratios (AL:GS) of 0.4 and 0.5, a reduction in compressive and flexural strength was observed in the case of geopolymer concrete with increasing FCC residue content. On the contrary, geopolymer concrete with increasing FCC residue content exhibited improved strength with an AL:GS ratio of 0.65. Relationships enabling estimation of geopolymer elastic modulus based on compressive strength were investigated. Scanning electron microscope (SEM) images and X-ray diffraction (XRD) patterns revealed that the final product from the geopolymerization process consisting of FCC residue was similar to fly ash-based geopolymer concrete. These observations highlight the potential of FCC residue as an aluminosilicate source for geopolymer products.