The nuclear spin-lattice relaxation rate 1/T1 is calculated for magnetic ring clusters by fully diagonalizing their microscopic spin Hamiltonians. Whether the nearest-neighbor exchange interaction J is ferromagnetic or antiferromagnetic, 1/T1 versus temperature T in ring nanomagnets may be peaked at kBT ≃ |J| provided the lifetime broadening of discrete energy levels is in proportion to T 3 . Experimental findings for ferromagnetic and antiferromagnetic Cu II rings are reproduced with crucial contributions of magnetic anisotropies as well as acoustic phonons. and therefore, serve to reveal a quantum-to-classical crossover between molecular and bulk magnets [6].Nuclear magnetic resonance (NMR) is an effective probe of low-energy spin dynamics, and the nuclear spinlattice relaxation time T 1 has been measured for various molecular wheels [7,8,9,10,11,12,13,14,15]. Interestingly, 1/T 1 as a function of temperature T under a fixed field H is commonly peaked at k B T ≃ |J|, where J is the intracluster exchange interaction between neighboring ion spins. Baek et al. [12] have recently provided a key to this long-standing problem by reanalyzing extensive observations of antiferromagnetic rings. When 1/T 1 is divided by the static susceptibility-temperature product χT , its peak is more pronounced and well-fitted to the Lorentzian-type expression,where ω N ≡ γ N H is the Larmor frequency of probe nuclei, whereas ω c is what they define as the temperaturedependent correlation frequency. The renormalized relaxation rate is thus peaked at a temperature satisfying ω c (T ) ≃ ω N (H). Considering the significant difference between the electronic and nuclear energy scales (hω N < ∼ 10 −5 |J|),hω c (T ) may be ascribed to the averaged lifetime broadening of discrete energy levels. Demonstrating that chromic and ferric wheels give ω c ∝ T α with α = 3.0 ∼ 3.5, Baek et al. claim that the exchangecoupled ion spins are likely to interact with the host molecular crystal through the Debye-type phonons.In response to this stimulative report, several authors [16,17] inquired further into the underlying scenario. While their arguments were elaborately based on microscopic spin Hamiltonians and enlighteningly verified the relevance of spin-phonon coupling to the notably peaked 1/T 1 , any magnetic anisotropy was neglected and/or most of the transition matrix elements were discarded in their evaluation of the dynamic spin correlation functions. Thus, we take the naivest but thus cumbersome approach: We set up realistically dressed Hamiltonians, completely diagonalize them, and sum up all the transition matrix elements into the dynamic structure factor. Such calculations are inevitably restricted to sufficiently small clusters but can nevertheless illuminate key factors in nanoscale spin dynamics, intrinsic intracluster anisotropies and extrinsic intercluster phonons.We consider both ferromagnetic and antiferromagnetic rings of various metal ion spins and describe them by the Hamiltonian |A στ q | 2 is the form factor describing the hyper...