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Magnetic and electronic properties of quantum materials heavily rely on the crystal structure even in the same chemical compositions. In this study, it is demonstrated that a layered tetragonal EuCd2Sb2 structure can be obtained by treating bulk trigonal EuCd2Sb2 under high pressure (6 GPa) and high temperature (600 °C). Magnetization measurements of the newly formed layered tetragonal EuCd2Sb2 confirm an antiferromagnetic ordering with Neel temperature (TN) around 16 K, which is significantly higher than that (TN ≈ 7 K) of trigonal EuCd2Sb2, consistent with heat capacity measurements. Moreover, bad metal behavior is observed in the temperature dependence of the electrical resistivity and the resistivity shows a dramatic increase around the Neel temperature. Electronic structure calculations with local density approximation dynamic mean–field theory (LDA+DMFT) show that this material is strongly correlated with well‐formed large magnetic moments, due to Hund's coupling, which is known to dramatically suppress the Kondo scale.