The proton and fluorine nuclear spin-lattice relaxation has been measured in FeSiFg • 6H2O in the temperature range 130 K ^ T ^ 420 K with standard pulse methods at 30 MHz. The relaxation times, T\(X H) and T\(19F), decrease with decreasing temperature according to the expression T\ = a (I) exp(-A/T) (I -1H, 19F). They show no significant dependence on the Larmor frequency. Thus, the unpaired Fe2+ electrons are mainly responsible for the proton and fluorine spin-lattice relaxation. The relaxation mechanism is described by an Orbach process. The ratio (19F)/7T i (*H) is relatively constant over the whole temperature range investigated. This is explained by the strong H ... F bonds in FeSiFß • 6H2O. The sharp increase of 71 i(1H) and T\ (19F) at 224 K is attributed to the phase transition, which probably alters the crystal field at the Fe2+ centers.