This work systematically investigates the impact of the dilute Sc addition on microstructures and mechanical properties in Mg alloys. Electron back scattered diffraction, slip traces analysis, transmission electron microscopy, and visco-plastic self-consistent polycrystal constitutive (VPSC) modeling were performed to investigate the deformation mechanisms in the tensile testing, especially the activation of <c+a> slip. The results showed that as-solid solution samples only consisted of α-Mg phase. After extrusion, all samples exhibited a similar average grain size. With the increment of the Sc content, the ductility of the samples was significantly improved, which failure elongation (FL) of Mg-xSc (x = 0.3, 0.6, 0.9 wt.%) alloys improved from 14.4% to 24.8%. The yield strength of each alloy is similar, about 200 MPa. VPSC results indicated that the difference value of the initial slip resistance (τ0) between prismatic slip and basal slip decreases from 63 MPa to 49 MPa, and the difference value of τ0 between pyramidal slip and basal slip decreases from 72 MPa to 57 MPa. The VPSC and the two-beam diffraction results confirmed that the pyramidal <c+a> slip and prismatic <a> slip were activated in tensile testing. The quantitative analysis of the slip trace line verified that the volume of non-basal slip reached 49.5% when the Sc content increased to 0.9 wt.%. Therefore, the addition of Sc in solid solution increased the amount of pyramidal <c+a> and prismatic <a> dislocation activities during the deformation process, which was beneficial to coordinate the c-axis strain, and finally improved ductility of Mg alloy.