Effects of solute segregation at grain boundaries (GBs) on the deformation mechanism and fracture behavior remain obscure for magnesium (Mg) alloys. Here, by introducing Zn segregation at GBs, we obtained an Mg-0.5Al-0.4Mn-0.2Ce-0.4Zn (wt.%) alloy achieving fracture elongation (FEL) of ∼33.6 %, with a remarkable FEL improvement by 100 % in comparison to Zn-free counterpart. Meanwhile, the tensile yield strength (TYS, 195.5 MPa) is increased by ∼27.5 MPa after trace Zn addition. Although trace Zn addition improves the fraction of GBs with high misorientation, it reconciles crack tolerance with enhanced strength. The introduction of Zn not only promotes pyramidal 〈c + a〉 slips and inhibits twinning nucleation, but also enhances the GB cohesion by Zn segregation. Based on in-situ microstructure observation, we found that the enhanced GB cohesion enables the segregation-inspired hierarchical crack buffering, as well as deflecting and branching. Enhanced GBs can also facilitate the continuous emission of 〈c + a〉 dislocations in neighboring grains irrespective of the onset of microcracks, forming a plastic zone to retard local strain concentration, thus avoiding microcrack percolation and attaining a crack-mediated elongation reserve of above 15 %. Besides, the higher TYS in the Zn-containing alloy mainly stems from the enhanced solid-solution strengthening of Zn solutes, thus achieving strength and crack tolerance synergy.