Several copper indium bimetallic single-source precursors (SSPs 2-9) have been prepared efficiently by exchange reactions of (Ph3P)(2)Culn(SEt)(4) (1) with protic ligands. This divergent approach has been successfully applied on multigram scales to produce nearly quantitative yields of known and newly reported SSPs. The former group features the previously difficult target (Ph3P)(2)Culn(SePh)(4) (2), and the latter includes (Ph3P)(2)Culn(SEt)(2)(SePh)(2) (3), the first SSP to incorporate both sulfur and selenium within a single copper indium bimetallic complex.