Double deprotonation of the salt [Ph2B(PMe3)(2)]-[OTf] (1) provides access to a bis(ylide)diphenylborate ligand that is readily transferred in situ to iron(II). Depending on the reaction stoichiometry, both the "ate" complex [Ph2B(Me2PCH2)(2)Fe(mu- Cl)(2) Li(THF)(2)] (2) and the homoleptic complex [Ph2B(Me2PCH2](2)Fe (3) can be prepared from FeCl2(THF)(1.5). Further reaction of 3 with FeCl2.(THF)1.5 produces the chloride-bridged dimer [Ph2B(Me2PCH2)(2)Fe(mu-Cl)(2) Fe(CH2PMe2)(2)BPh2](4). At- tempts to reduce or alkylate 4 provide 3 as the only isolable product, likely a consequence of the low steric hindrance of the bis(ylide)diphenylborate ligand. On the other hand, reaction of 4 with the strong field ligand (CNBu)-Bu-t provides the six-coordinate, diamagnetic complex [Ph2B(Me2PCH2)(2)Fe((CNBu)-Bu-t)(4)][Cl](5). Electronic structure calculations for the bis(ylide)diphenylborate ligand and homoleptic complex 3 suggest that the C(ylide) atoms are strong sigma-donors with little pi-bonding character. These initial results suggest the potential for this bis(ylide)diphenylborate ligand in coordination chemistry.