The electron precise [Mo3(μ3-S)(μ-S)3(dppe)3Br3]+ incomplete cuboidal complex with six cluster skeletal electrons (CSE) can be converted to the paramagnetic bicapped [Mo3(μ3-S)2(μ-S)3(dppe)3]+ cluster with an unusual seven metal electron population by treatment with tBuSNa, which simultaneously serves as a reducing agent and a source of the additional capping sulfur atom.