Experimental and computational studies on PPh3 and PCy3-substituted ylide-functionalized phosphines as well as on a biaryl and a cyclohexyl-aryl phosphine demonstrate that Au⋅⋅⋅H−C hydrogen bonds can serve as secondary metal ligand interactions similar to gold–arene interactions often used in ligand design for the stabilization of catalytically active species. Remarkably short Au−H bonds are observed.