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Abstract While ∼30% of materials are reported to be topological, topological insulators are rare. Magnetic topological insulators (MTI) are even harder to find. Identifying crystallographic features that can host the coexistence of a topological insulating phase with magnetic order is vital for finding intrinsic MTI materials. Thus far, most materials that are investigated for the determination of an MTI are some combination of known topological insulators with a magnetic ion such as MnBi₂Te₄. Motivated by the recent success of EuIn₂As₂, the role of chemical pressure on topologically trivial insulator is investigated, Eu₅In₂Sb₆via Ga substitution. Eu₅Ga₂Sb₆is predicted to be topological but is synthetically difficult to stabilize. The intermediate compositions between Eu₅In₂Sb₆and Eu₅Ga₂Sb₆are observed through theoretical works to explore a topological phase transition and band inversion mechanism. The band inversion mechanism is attributed to changes in Eu–Sb hybridization as Ga is substituted for In due to chemical pressure. Eu₅In_4/3Ga_2/3Sb₆is also synthesized, the highest Ga concentration in Eu₅In_2‐xGa_xSb₆, and report the thermodynamic, magnetic, transport, and Hall properties. Overall, the work paints a picture of a possible MTI via band engineering and explains why Eu‐based Zintl compounds are suitable for the co‐existence of magnetism and topology.