In recent years, there has been a growing interest in one-part alkali-activated materials, which utilize solid-form alkali activators, within the construction industry. This approach is becoming popular due to its simpler and safer application for cast-in-situ purposes, as compared to the conventional two-part method. At this purpose, we have pioneered the use of volcanic deposits of Mt. Etna volcano (Italy) as precursor for the synthesis of a unique one-part formulation. This was done to assess its performance against both traditional and two-part alkali-activated materials. The study employed a comprehensive range of investigative techniques including X-ray powder diffraction, Fourier transform infrared spectroscopy, hydric tests, mercury intrusion porosimetry, ultrasound, infrared thermography, spectrophotometry, contact angle measurements, uniaxial compressive strength tests, as well as durability tests by salt crystallization and freeze–thaw cycles. The key findings on the studied samples are as follows: i) small size of pores and slow absorption-drying cycles; ii) satisfying compactness and uniaxial compressive strengths for building and restoration interventions; iii) high hydrophily of the surfaces; iv) lower heating dispersion than traditional materials; v) significant damage at the end of the salt crystallization test; vi) excellent resistance to freeze–thaw cycles. These newly developed materials hold promises as environmentally friendly options for construction applications. They offer a simplified mixing process in contrast to the conventional two-part alkali-activated materials, thus providing an added advantage to this class of materials.