We investigate bulk poly(propyleneimine) dendrimers of generation (G) 2-5 by dielectric spectroscopy (DS), solid-state H-2 NMR, and field-cycling H-1 NMR relaxometry (FC H-1 NMR) in a large temperature range (120-400 K). Three relaxation processes are identified by DS: a main (alpha-) relaxation (T > T-g) and two secondary processes (T < T-g). The a-process exhibits a sup er-Arrhenius temperature dependence typical of glass-forming liquids and changes only weakly with G, yielding T-g similar to 200 K. The temperature dependence of the secondary relaxations is governed by an Arrhenius law. While one secondary process exhibits features characteristic for glasses, the other is atypical. Its time constant is virtually independent of G, and its spectral width does not increase with lowering temperature as is usually observed for sub-T-g relaxations. Regarding FC H-1 NMR probing the dispersion of the spin lattice rate R-1 in the frequency range 200 Hz-30 MHz, transformation to the susceptibility representation, chi ''(omega) omega R-1(omega), and applying frequency-temperature superposition, an effective frequency range of 9 decades is covered by a master curve chi ''(omega tau(alpha)). In addition to the segmental time tau(alpha)(T), which complements the results from DS up to high temperatures, a longer terminal relaxation tau(t)(T) is identified. In between, an intermediate power-law regime is observed in chi ''(omega tau(alpha)) with an exponent of about 0.8. The broad relaxation spectrum is attributed to local dynamics, breathing modes, and overall tumbling and diffusion of the dendrimer molecule. In the low-frequency limit, R-1(omega) is determined by intermolecular relaxation from which the molar mass dependence of the translational diffusion coefficient can be estimated. We find D(M) proportional to M-1.2 +/- 0.2.