Boron nitride (BN) aerogels are three-dimensional bulk materials with exceptional performances in a wide range of areas. However, detailed investigations into the relationship of synthesis, structure, and properties are rare. This study demonstrates the feasibility of tuning the performance of the aerogel by simply altering the relative amount of the precursors in the synthesis, which subsequently leads to the formation of aerogels with distinctive properties such as specific surface areas, porosity, and compressibility. The applications of these structurally different aerogels are exemplified by investigating in a series of important industrial-related areas, such as oil absorption/desorption, direct combustion, adsorptive desulfurisation, and CO2 capture. The study raises the application prospects of BN aerogels in gas-phase catalysis and thermal superinsulation materials.