We present the magnetic properties of three recently synthesized binuclear molecular complexes [NiNd], [NiGd], and [ZnGd] investigated by dc magnetization and proton nuclear magnetic resonance (NMR) measurements. The high-temperature magnetic properties are related to the independent paramagnetic behavior of the two magnetic metal ions within the binuclear entities both in [NiNd] and [NiGd]. On lowering the temperature, the formation of a magnetic dimer, with a low-spin ground state due to antiferromagnetic interaction ($J$/${k}_{B}$ \ensuremath{\approx} \ensuremath{-}25 K) between Ni${}^{2+}$ and Nd${}^{3+}$, is found in the case of [NiNd], while in [NiGd], a ferromagnetic interaction ($J$/${k}_{B}$ \ensuremath{\approx} 3.31 K) between the magnetic ions leads to a high-spin ($S$ $=$ 9/2) ground state. The temperature dependence of the proton nuclear spin lattice relaxation rate ${T}_{1}$${}^{\ensuremath{-}1}$ in [NiNd] is driven by the fluctuation of the hyperfine field at the nuclear site due to relaxation of the magnetization. At high temperatures, the independent Ni${}^{2+}$ and Nd${}^{3+}$ spins fluctuate fast, while at low temperatures, we observe a slowing down of the fluctuation in the total magnetization of the dimer because of the insurgence of antiferromagnetic spin correlations. The relaxation mechanism in [NiNd] at low temperatures is interpreted by a single temperature-dependent correlation frequency ${\ensuremath{\omega}}_{\mathrm{c}}$ \ensuremath{\propto} ${T}^{3.5}$, which reflects the lifetime broadening of the exchange-coupled spins via spin-phonon interaction. The proton NMR signal in [NiGd] could just be detected at room temperature due to the shortening of relaxation times when $T$ is decreased. The magnetic properties of [ZnGd] are the ones expected from a weakly interacting assembly of isolated moments except for anomalies in the susceptibility and NMR results below 15 K, which currently cannot be explained.