Treatment of the [2‐Cp‐9‐tBuNH‐closo‐2,1,7,9‐FeC3B8H10] (1) ferratricarbollide (Cp = η5‐C5H5−) with Na+ C10H8− in 1,2‐dimethoxyethane (DME) at room temperature produced an air‐sensitive transient anion with a tentatively identified nido‐[tBuNH‐CpFeC3B8H10]2− constitution. In‐situ reaction of this low‐stability ion with [CpFe(CO)2I] or [CpFe(CO)2]2 generated three violet diferratricarbaboranes identified as paramagnetic subcloso complexes [4,5‐Cp2‐‐4,5,1,6,7‐Fe2C3B8H11] (2; yield 2 %), [4,5‐Cp2‐‐4,5,1,7,12‐Fe2C3B8H11] (3; yield 2 %), and [7‐tBuNH‐4,5‐Cp2‐‐4,5,1,7,12‐Fe2C3B8H10] (4; yield 14 %). These first representatives of the 13‐vertex dimetallatricarbaborane family were characterized by EPR and IR spectroscopy, and mass spectrometry, and their structures were determined by X‐ray diffraction analysis.