A systematic evaluation of the accuracy of the GROMOS-compatible 2016H66 force field in the simulation of dendrimers is performed. More specifically, the poly(amido amine) (PAMAM) and the poly(propyleneimine) (PPI) are considered because of the availability of experimental data and simulation results in the literature. A total of 36 molecular systems are simulated and the radius of gyration, asphericity, density profiles, and the self-diffusion coefficient are monitored in terms of the generation number and pH (low, medium, and high) condition. Overall, the results support the recommendation of the 2016H66 force field for the simulation of dendrimer systems. The natural building-block based strategy adopted in the definition of 2016H66, together with a careful parametrization of the chemical functional groups to reproduce thermodynamic properties in environments of different polarity, and also the ability to accurately reproduce the expected structural and dynamic features of dendrimers, as shown in the present work, make this force field an attractive option for the simulation of such systems.