• A synergistic grain-refining strategy is introduced to control the structure of Al-Zn-Mg-Cu alloy. • The LPBF processability of the Al-Zn-Mg-Cu alloy is increased by grain refinement. • The UTS and EL of Al-Zn-Mg-Cu-Ti-TiC alloy are way above those of Al-Zn-Mg-Cu alloy. • The underlying grain refinement mechanism of different grain refiners is discussed. Grain refinement is critical to surpassing the bottlenecks of inherent hot tearing of high-strength aluminum alloys fabricated by additive manufacturing (AM). In this study, a synergistic grain-refining strategy including heterogeneous nucleation, solute-driven growth restriction and nanoparticle-induced growth restriction was introduced to control the microstructure of Al-Zn-Mg-Cu alloys during the laser powder bed fusion (LPBF) process. Crack-free Al-Zn-Mg-Cu alloys with significantly refined grains were safely fabricated via LPBF by coincorporation of TiC and TiH 2 particles. In-situ L1 2 -Al 3 Ti particles were produced to promote the heterogeneous nucleation. The grain growth was restricted by adding Ti solute, while introduced TiC nanoparticles (NPs) improved the density of heterogeneous nucleation sites and blocked grain growth physically. The resultant elimination of columnar grains and hot cracks in the (1 wt.%) TiC- and (0.8 wt.%) TiH 2 -modified Al-Zn-Mg-Cu alloy resulted in excellent ultimate tensile strength (UTS) of 593 ± 24 MPa, yield strength (YS) of 485 ± 41 MPa and elongation (EL) of 10.0% ± 2.5% under the T6 condition. This study provides new insights into improving the grain microstructure and mechanical properties of high-strength aluminum alloys during LPBF.