Traditional thermochemical synthesis of N-containing compounds presents disadvantages in terms of high energy consumption and large pollution, motivating growing interest in the development of energy-saving, efficient, and green electrochemical alternatives. Due to their special structure and electronic properties, amorphous nanomaterials possess several advantages for applications in catalysis, which include electrochemical synthesis of N-containing compounds. This paper reviews recent research progress in the application of amorphous nanomaterials as electrocatalysts for efficient electrosynthesis of N-containing compounds from a variety of abundant N-containing small molecules (N2, NO, NO3−, etc.). It discusses the controllable synthesis and structural advantages of amorphous nanomaterials and their enhanced electrocatalytic properties for various N-containing systems with emphasis on the structure-function relationships between the catalysts and catalytic reactions, especially for the p orbital regulated main group catalysts. Finally, it makes recommendations for future electrochemical synthesis of various N-containing compounds and describes current challenges as well as opportunities for new developments.