We demonstrate and thoroughly examine tobacco mosaic virus (TMV)-templated palladium (Pd) nanocatalysts for the ligand-free Suzuki coupling reaction under mild conditions. The surface-assembled TMV templates allow for facile catalyst synthesis under mild aqueous conditions that leads to high Pd surface loading and stability. Further, the chip-based format enables simple catalyst separation and reuse as well as facile product recovery. Reaction condition studies demonstrated that the solvent ratio played an important role in the selectivity of the Suzuki reaction, and that a higher water/acetonitrile ratio significantly facilitated the cross-coupling pathway. We envision that our viral template-based bottom-up assembly approach can be readily extended to other biotemplates, metal catalysts and organic reaction systems.