Two birds, one nanoparticle: A highly efficient and selective tandemreaction comprising CN and CC cross‐coupling of iodoanilines to form styrylguanidines by using a recyclable, heterogeneous, supported palladium nanoparticle catalyst is reported (see scheme). A mechanistic proposal based on coordination of palladium nanoparticles to the basic N atoms of aniline and guanidine is supported by isolation