Triarylborane Lewis acids bind [Fe-2(pdt)(CO)(4)(CN)(2)](2-) [1](2-) (pdt(2-) = 1,3-propanedithiolate) and [Fe-2(adt)(CO)(4)(CN)(2)](2-) [3](2-) (adt(2-) = 1,3-azadithiolate, HN(CH2S-)(2)) to give the 2:1 adducts [Fe-2(xdt)-(CO)(4)(CNBAr3)(2)](2-). Attempts to prepare the 1:1 adducts [1(BAr3)](2-) (Ar = Ph, C6F5) were unsuccessful, but related 1:1 adducts were obtained using the bulky borane B(C6F4-o-C6F5)(3) (BArF*(3)). By virtue of the N-protection by the borane, salts of [Fe-2(pdt)(CO)(4)(CNBAr3)(2)](2-) sustain protonation to give hydrides that are stable (in contrast to [H1](-)). The hydrides [H1(BAr3)(2)](-) are 2.5-5 pK(a) units more acidic than the parent [H1](-). The adducts [1(BAr3)(2)](2-) oxidize quasi-reversibly around -0.3 V versus Fc(0/+) in contrast to ca. -0.8 V observed for the [1]2(-/-) couple. A simplified synthesis of [1](2-), [3](2-), and [Fe-2(pdt)(CO)(5)(CN)](-) ([2](-)) was developed, entailing reaction of the diiron hexacarbonyl complexes with KCN in MeCN.