Copper slag (CS) remains a challenging industrial by-product with a relatively small utilization fraction. The present study investigated the development of one-part alkali-activated cements based on CS, ground granulated blast furnace slag (GGBS) and a mixture of the two as a precursor. We investigated 5 to 15 wt% solid sodium metasilicate (Na2SiO3) and disilicate (Na2Si2O5) as alkaline reagents. Isothermal calorimetry showed that the reactivity of the system was higher for the metasilicate based samples, with early reaction and higher cumulative heat released. Metasilicate based samples also presented a more densified microstructure, lower porosity and higher strength. Better performances were observed with 10 wt% metasilicate/disilicate with respect to the 5 and 15 wt%. The 28-day compressive strength and elastic modulus of 10 wt% metasilicate samples reached 75 MPa and 25 GPa, respectively, and, for paste samples, ranged from 100 wt% GGBS to 50/50 wt% CS/GGBS. The microstructure and calorimetry of the pastes showed that GGBS actively participated in the binding process, whereas CS played a smaller role and acted as a filler and catalyst. The substitution of commercial GGBS by CS up to 50 wt% did not affect the overall performance, thus, bringing CS forward as an economically interesting precursor.