A single crystal of iron (II) carbohydrazide perchlorate [FeII (CHZ)3](ClO4)2 (FeCP), a novel, lead-free, energetic coordination compound, was synthesized and its structure determined by X-ray single crystal diffraction for the frst time. The crystal belongs to the monoclinic system P2(1)/n space group, with a = 1.0066(2) nm, b = 0.8458(2) nm, c = 2.1194(4) nm, β = 100.693(3)° and Z = 4. The central Fe(II) ion is coordinated to three bidentate carbohydrazide units through the carbonyl oxygen atom and an amino nitrogen atom, forming a six-coordinated, non-centrosymmetric complex cation. The thermal analyses by differential scanning calorimetry and thermogravimetry show that the onset temperature of thermal decomposition (152.7 °C) and the critical temperature of thermal explosion of FeCP (161.2 °C) are both much lower than those of other transition metal carbohydrazide perchlorate compounds, and also those of some other primary explosives in service. FeCP has a high enthalpy of combustion, as measured by oxygen bomb calorimetry. The impact, friction and fame sensitivity tests indicate that FeCP is extremely sensitive and hazardous. Unexpected explosions occurred even during the operational processes. In order to explore the intrinsic cause of these explosions, theoretical calculations of the orbital energies were performed based on DTF. These results reveal that the impact sensitivity is positively correlated with the energy gap between HOMO and LUMO: the smaller energy gap results in the higher impact sensitivity.