Cement is a fundamental component in construction, providing the binding matrix for concrete, mortar, and other building materials. However, traditional cement production contributes significantly to carbon emissions and energy consumption, prompting the exploration of alternative formulations to enhance sustainability without compromising performance. This research investigates the enhancement of cement paste properties through alkali activation using vermiculite powder, calcium aluminate cement (CAC), and ground granulated blast furnace slag (GGBFS). Alkali activation is a promising approach for improving the performance of cementitious materials, offering benefits such as increased strength. Vermiculite, known for its high caution exchange capacity and thermal stability, is explored as a supplementary cementitious material in this study. Various cement paste formulations were prepared, incorporating different proportions of vermiculite powder, CAC, and GGBFS. The effects of these formulations on compressive strength were evaluated at 7, 14, and 28 days using a sodium hydroxide (NaOH) solution as the activating agent. Specimens measuring 50 mm × 50 mm × 50 mm were prepared with a composition of 50% GGBFS, 25% vermiculite powder, and 25% calcium aluminate cement. The results demonstrate significant improvements in compressive strength over time. At 7 days, the formulations achieved compressive strengths of 14 MPa, 15 MPa, and 18 MPa, respectively. These strengths continued to increase at 7, 14, and 28 days, indicating the effectiveness of alkali activation in enhancing the properties of the binder.