Transition metal catalysis employing disilanes and silylboranes for synthesizing organosilanes circumvents the limitations of conventional hydrosilylations. While disilanes require special conditions, silylboranes have yet to be developed as TMS sources. Functional group compatibility renders silylzinc reagents desirable; however, their development is hindered by their synthesis using pyrophoric silyllithium and dissolved lithium salts. Our solid Me3SiZnI circumvents these limitations and herein, we demonstrate its significance in the cross‐coupling of aryl and alkyl bromides.