Synthesis of the lithium salt of the bis(imido) organoarsenate dianion was investigated that cocomplexes n-butyllithium to give a complex. It was observed that the signal of the NH resonance in both the infrared radiation (IR) and H nuclear magnetic resonance (NMR) spectra was unavailable indicating that full metallation of the amide protons had occured. The H NMR spectrum showed several multiplets in the low frequency region that was used to show the presence of alkyl groups. A low-temperature X-ray crystallographic investigation of the product showed it to be an ion-contacted dimeric structure that comprises of two dianions and two monoanions linked together by six lithium cations.