Cellulose nanofibrils (CNFs) have been proposed as reinforcement for thermoplastic polymers due to their potentially superior mechanical properties. However, it seems still uncertain how the reinforcement ability of CNFs compares to cheaper pulp fibres, and how the suspected potential of CNFs can be fully utilized in biocomposites. Therefore, this study presents a direct comparative investigation of kraft pulp fibres and their fibrillated materials as reinforcement of high- or low-density polyethylene. Besides the experimental investigations, the tensile properties of the corresponding biocomposites were predicted by using micromechanical analysis. It was shown that considering the same fraction of fibrous materials (pulp fibres vs CNFs), the experimental and modelling results revealed that the highest tensile strength was obtained from the pulp fibre-reinforced biocomposites. Regarding the CNFs-reinforced biocomposites, the compatibilizer content had to be up to 20 wt% to experimentally achieve the tensile strength predicted by the model. © 2023 The Author(s)