This study focuses on the use of alkali-activated materials and geopolymer grouts in deep soilmixing. Three types of grouts, incorporating metakaolin and/or slag and activated with sodium silicate solution, were characterized at different scales to understand the development of their local structure and macroscopic properties. The performance of the soilmix was assessed by using combinations of the grouts and model soils with different clay contents. Feret’s approach was used to understand the development of compressive strength at different water-to-solid ratios ranging from 0.65 to 1. The results suggested that incorporating calcium reduced the water sensitivity of the materials, which is crucial in soilmixing. Adding soils to grouts resulted in improved mechanical properties, due to the influence of the granular skeleton. Based on strength results, binary soilmix mixtures containing 75% of metakaolin and 25% of slag, with H2O/Na2O ratios ranging from 28 to 42 demonstrated potential use for soilmixing due to the synergistic reactivity of metakaolin and slag. The optimization of compositions is necessary for achieving the desired properties of soil mixtures with higher H2O/Na2O ratios.