AbstractCement production is responsible for 5%–7% of global CO2 emissions, highlighting the need for sustainable alternatives like geopolymer composite (GCOMP) to meet the growing demand for concrete. This study investigates the mechanical, microstructural, and thermal properties of GCOMP by incorporating nano‐alumina (n‐alumina) and MSF (MSF). The n‐alumina content was varied at 1%, 2%, and 3% by weight of the mix, while the MSF content remained fixed at 0.5% by weight. Thermal characterization was conducted up to 800°C. The performance of GCOMP blends with n‐alumina was compared to a control blend consisting of only 0.5% MSF. Various mechanical properties were evaluated for all GCOMP blends. Microstructural and mineralogical characteristics were analyzed using scanning electron microscopy (SEM), X‐ray diffraction (XRD), and Fourier‐transform infrared spectroscopy (FTIR). Thermogravimetric and differential thermal analysis were performed up to 800°C for the thermal analysis of the GCOMP mix. The results indicate that the optimal mechanical properties were achieved with 2% n‐alumina (compressive and flexural strength increased by 35.65% and 77.7%, respectively). Additionally, the incorporation of n‐alumina improves the interfacial zones and results in a denser structure. GCOMP mortars portrayed a mass loss between 25°C and 250°C, with a marginal mass loss occurring between 250°C and 715°C. No mass loss was observed between 715°C and 800°C. The MSF‐reinforced GCOMP mortars experienced an ultimate mass loss of approximately 12%, with the MSF showing negligible influence. The addition of n‐alumina particles to MSF‐reinforced GCOMP resulted in the development of stronger samples characterized by the presence of C–S–H, calcium aluminate oxide hydroxide, and quartz.