Brownleeite, ideally stoichiometric MnSi, is a manganese silicide not previously observed in nature that was discovered within an interplanetary dust particle that likely originated from a comet. Three submicrometer brownleeite grains were found, with one of them poikilitically enclosed by Mnbearing forsterite. Owing to the small size of the brownleeite grains, it was not possible to determine conventional macroscopic properties of this mineral; however, the chemical composition and crystal structure were well constrained by extensive quantitative energy dispersive X-ray analysis and electron diffraction using transmission electron microscopy (TEM). The crystal system for brownleeite is cubic (a = 4.557 Å) with space group P2 1 3, cell volume = 94.63 Å 3 , Z = 4, density (calculated) = 2.913 g/cm 3 , and empirical formula: (Mn 0.77 Fe 0.18 Cr 0.05 )Si. These brownleeite grains likely formed as high-temperature condensates either in the early Solar System or in the outflow of an evolved star or supernova explosion.