Grounded in the auspicious horizons of geological polymers as alternative replacements for Portland cement and aligned with the national endeavor of constructing an ecological civilization and harnessing solid waste as a resource, this study delves into the integration of nanostructured calcium carbonate (CaCO3) into geological polymers derived from fly ash and manganese slag. Employing a comprehensive methodology involving modalities, such as X-ray diffraction, scanning electron microscopy, and attenuated total reflectance Fourier-transform infrared spectroscopy, the influence of nano-CaCO3 on the compressive strength, pore architecture, and polymerization degree of geological polymers is meticulously unveiled. The outcomes reveal that nano-CaCO3 adeptly infiltrates the intricate microporous architecture of geological polymers, thereby providing a compact and intrinsically reinforcing matrix, ultimately endowing a marked increase in compressive strength. The assimilation of nano-CaCO3 correlates conspicuously with an increase in monomeric calcium concentrations, thereby catalyzing and expediting the formation of polymeric assemblages within the system, which in turn accelerates the progression of geological polymerization. This catalytic effect augments the intricate three-dimensional lattice-like gel structures, consequently orchestrating a substantial amelioration in mechanical attributes. When the dosage of nano-CaCO3 was 3.5%, sodium silicate was 10%, and NaOH was 12%, the integrated performance of fly ash–Mn slag geopolymer was optimal. Specifically, the 28-day compressive strength reached 25.6 MPa, and the compressive strength of the weathering performance test increased by 8.31%. The polymer achieved 96.77% curing of Mn, and it was non-radioactive. Thus, the prepared geopolymers are safe and reliable and support the subsequent development of nanomaterial activators.