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This paper reviews the recent work carried out in the field of modern high-energy materials (HEMs) with the emphasis on homoleptic polynitrogen compounds. A large volume of quantum-chemical investigations have predicted the possibility of existence of polynitrogen compounds not only as short-lived transient species but also in the form of isolable discrete molecules. Despite the theoretical speculations, only a few polynitrogen ions are known today in addition to well-entrenched Ndiscovered almost 100 year ago. Extraordinary potential of these green molecules to deliver high amounts of energy in comparison with today’s and tomorrow’s most powerful HEMs, namely, hexanitrohexaazaisowurtzitane (CL-20) and octanitrocubane (ONC), has fuelled the imagination of propellant and explosive engineers and technologists. Research activities are in progress in many quantum-chemical schools to explore the possibility of other promising polynitrogen compounds. After the recent discovery of key synthons/building blocks Mg(N5)2, NSbF, NSbF11, N, NSnF6, and NSn(CF3)4, the wealth of polynitrogen compounds is just waiting to be harvested by the HEMs community. There are ambitious plans all over the globe to realize N60, which only prove a eco-friendly dense powerhouse of energy. [ABSTRACT FROM AUTHOR]