We report the temperature dependence of the spin dynamics of the octacyanometallates [Mo(CN)8]3- and [W(CN)8]3-. At 5 K, these complexes display remarkably long spin-lattice relaxation times of 1.05 s, and 0.63 s, respectively. We probe the contributing factors to the spin relaxation and demonstrate the impact of spin-orbit coupling as a handle to tune vibrationally mediated spin-lattice relaxation.