Abstract The finding of the unprecedented 16‐e tricoordinate planar rhodium(−Ι) complex, K[Rh(IPr)(dvtms)] (K[ 1 ]) (IPr = 1,3‐bis(2,6‐diisopropylphenyl)imidazolyl‐2‐ylidene, dvtms = divinyltretramethyldisiloxane) prompted us to explore its reactivity. K[ 1 ] reacts as a nucleophile with methyliodide to give [Rh(IPr)(dvtms)Me], a Rh(Ι) compound with an exceptional trigonal‐pyramidal structure. Other haloalkanes abstract one electron from K[ 1 ] to give the previously reported [Rh 0 (IPr)(dvtms)] complex. K[ 1 ] also reacts with protonic acids and weak proton sources such as water and ketones to eventually give the rare tricoordinate 14‐electron complex [Rh I (IPr)(SiMe 2 OSiMe 2 CH = CH 2 )] with a Rh −Si bond. The 16‐electron complex [Rh I (IPr)(SiMe
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