The strength of ultra-low carbon maraging stainless steels can be significantly enhanced by precipitating nanoscale intermetallic secondary phases. Retained or reversed austenite in the steel can improve its toughness, which is key to achieving an ideal combination of strength and toughness. Ti and Al are often used as cost-effective strengthening elements in maraging stainless steels but the synergistic toughening and strengthening mechanisms of Ti and Al have not been studied. To investigate the synergistic toughening and strengthening mechanisms of Ti and Al in Co-free maraging stainless steels, this paper focuses on the microstructure and mechanical properties of three alloys: Fe-12Cr-11Ni-1.7Al-0.5Ti (Steel A), Fe-12Cr-11Ni-0.5Ti (Steel B), and Fe-12Cr-11Ni-1.7Al (Steel C). The impact of Ti and Al on the microstructure and mechanical properties was investigated using X-ray diffraction (XRD), high-resolution transmission electron microscopy (TEM), and thermodynamic simulations. The relationship between microstructure, strength, and toughness is also discussed. The results indicated that Steel A, containing both Al and Ti, exhibited the highest strength level after solution treatment at 900 °C, with an ultimate tensile strength reaching 1571 MPa after aging at 540 °C. This is attributed to the simultaneous precipitation of spherical β-NiAl and rod-shaped η-Ni₃Ti phases. Steel B, with only Ti, formed a significant amount of Ni-rich reversed austenite during aging, reducing its ultimate tensile strength to 1096 MPa. Steel C, with only Al, showed a high strength–toughness combination, which was achieved by forming dispersive nano-sized intermetallic precipitates of β-NiAl in the martensitic matrix with a slight amount of austenite. It is highlighted that Al has superior toughening and strengthening effects compared to Ti in the alloy system.