[NiBr[subscript 2](PPh[subscript 3])[subscript 2]] and [NiBr[subscript 2](dppe)] are prepared from nickel bromide hydrate and phosphine. These brightly colored coordination compounds are then converted into the related organometallic compounds "trans"-[NiBr(Mes)(PPh[subscript 3])[subscript 2]] and [NiBr(Mes)(dppe)] (Mes = 2,4,6-Me[subscript 3]C[subscript 6]H[subscript 2]) by reaction with the Grignard reagent MesMgBr. Characterization of the compounds is accomplished by a combination of UV-vis and multinuclear NMR spectroscopies. [NiBr(Mes)(dppe)] is a highly active precatalyst for the Suzuki-Miyaura cross-coupling of 4'- bromoacetophenone and phenylboronic acid. The catalytic reaction is complete in as little as 15-20 min with only a 1 mol % precatalyst loading, and the reaction can be carried out in air. Results are assessed by [superscript 1]H NMR spectroscopy, or the solid 4-acetylbiphenyl product can be isolated following aqueous workup and recrystallization. The experiments are flexible and accommodate a variety of laboratory schedules and student skill levels. Each experimental component has been designed to be completed within a 3 h laboratory period.