Measurements of proton Nuclear Magnetic Resonance ( 1 H NMR) spectra and relaxation and of Muon Spin Relaxation (µ + SR) have been performed as a function of temperature and external magnetic field on two isostructural lanthanide complexes, Er(trensal) and Dy(trensal) (where H 3 trensal=2,2',2''-tris-(salicylideneimino)triethylamine) featuring crystallographically imposed trigonal symmetry. Both the nuclear 1/T 1 and muon λ longitudinal relaxation rates, LRR, exhibit a peak for temperatures T<30K, associated to the slowing down of the spin dynamics, and the width of the NMR absorption spectra starts to increase significantly at T∼50K, a temperature sizably higher than the one of the LRR peaks. The LRR peaks have a field and temperature dependence different from those previously reported for all Molecular Nanomagnets.. They do not follow the Bloembergen-Purcell-Pound scaling of the amplitude and position in temperature and field and thus cannot be explained in terms of a single dominating correlation time τ c determined by the spin slowing down at low temperature. Further, for T<50K the spectral width does not follow the temperature behavior of the magnetic susceptibility χ. We suggest, using simple qualitative considerations, that the observed behavior is due to a combination of two different relaxation processes characterized by the correlation times τ LT and τ HT , dominating for T<30K and T>50K, respectively. Finally, the observed flattening of LRR for T<5K is suggested to have a quantum origin.