One of the specific subjects in frustrated magnetic systems is the phenomenon coupled with noncollinear magnetism, such as zero or negative thermal expansion (ZTE or NTE) in antiperovskite compounds. The first-principles calculations and neutron powder diffraction (NPD) are used to reveal the control of the noncollinear Γ5g antiferromagnetic (AFM) structure and corresponding thermal expansion properties in Mn3Zn0.875X0.125N (X = Mn, Ge, and Sn). Based on the optimal exchange-correlation functional, our results demonstrate that X (X = Mn, Ge, and Sn) doping at Zn site could stabilize the noncollinear Γ5g AFM structure and produce magnetovolume effect (MVE). The predictions of Γ5g AFM ground state and MVE is further verified by the NPD results of Mn3Zn0.83Mn0.15N0.99. Intriguingly, this special magnetic structure with strong spin–lattice coupling can be tunable to achieve ZTE behavior. On the basis of these results we suggest that frustrated magnetic systems with noncollinear Γ5g AFM structure of Mn atoms i...