This work presented the production and incorporation of calcium-hydrolyzed nano-solutions at three concentrations (1, 2, and 3 wt.%) in alkali-activated gold mine tailings (MTs) from Arequipa, Perú. As the primary activator solution, a sodium hydroxide (NaOH) solution at 10 M was used. Calcium-hydrolyzed nanoparticles with a particle size of 10 nm were localized inside self-assembled molecular spherical systems (micelles) with diameters of less than 80 nm that were well-dispersed in aqueous solutions and acted as secondary activator, and also as additional calcium resource for alkali-activated materials (AAMs) based on low-calcium gold MTs. High-resolution transmission electron microscopy/energy-dispersive X-ray spectroscopy (HR-TEM/EDS) analyses were carried out to characterize the morphology, size, and structure of the calcium-hydrolyzed nanoparticles. Fourier transform infrared (FTIR) analyses were then used to understand the chemical bonding interactions in the calcium-hydrolyzed nanoparticles and in the AAMs. Scanning electron microscopy/energy-dispersive X-ray spectroscopy (SEM/EDS) and quantitative X-ray diffraction (QXRD) were performed to study the structural, chemical, and phase compositions of the AAMs; uniaxial compressive tests evaluated the compressive strength of the reaction AAMs; and nitrogen adsorption–desorption analyses measured porosity changes in the AAMs at the nanostructure level. The results indicated that the main cementing product generated was amorphous binder gel with low quantities of nanostructured C-S-H and C-A-S-H phases. The surplus production of this amorphous binder gel produced denser AAMs at the micro-level and nano-level (macroporous systems). In addition, each increase in the concentration of calcium-hydrolyzed nano-solution had a direct/proportional effect on the mechanical properties of the AAM samples. AAM with 3 wt.% calcium-hydrolyzed nano-solution had the highest compressive strength, with a value of 15.16 MPa, which represented an increase of 62% compared with the original system without nanoparticles that were aged under the same conditions at 70 °C for seven days. These results provided useful information about the positive effect of calcium-hydrolyzed nanoparticles on gold MTs and their conversion into sustainable building materials through alkali activation.