Polymeric materials are widely used in structural components and systems, and the accurate prediction of their complex time‐dependent behavior is critical. Several constitutive models are available for different types of mechanical behaviors and loading conditions. However, selecting the model and the correct calibration of its parameters is often a challenge. This paper evaluates the applicability of the two‐layer viscoplasticity (TLV) model to predict the viscoplastic behavior of polyvinylidene fluoride (PVDF) in a large range of strain rates and complex states of strain. The setting of parameters and model validation was made by performing experimentally and numerically uniaxial compression tests and relaxation tests. The model parameters were also analyzed in performing microindentation tests. The TLV model using the same set of parameters selected well predicted the PVDF behavior in a wide variety of compressive loading conditions. Experimental data compression test.