Synthesis, characterization, and thermolysis studies of new polynitro compounds with good oxygen balance are reported. These compounds have been fully characterized by IR, NMR, elemental analysis, differential scanning calorimetry (DSC), density, and impact sensitivity measurements. Additionally, the structure of 2,2,2-trinitro-N-2,2,2-trinitroethylidene-ethanamine (9) was confirmed by single-crystal X-ray diffraction. Based on experimental and calculated values, the properties of the new polynitro compounds, such as decomposition temperatures (102.7–154.4 °C), oxygen balance (−26.7–30.5%), detonation pressures (21.4–36.1 GPa) and velocities (7368–8749 ms⁻¹), and impact sensitivities (3–29 J), were obtained.