The FP7 EURATOM project FREYA has been executed between 2011 and 2016 with the aim of supporting the design of fast lead-cooled reactor systems such as MYRRHA and ALFRED. During the project, a number of critical experiments were conducted in the VENUS-F facility located at SCKCEN, Mol, Belgium. The Monte Carlo code Serpent was one of the codes applied for the characterization of the critical VENUS-F cores. Four critical configurations were modeled with Serpent, namely the reference critical core, the clean MYRRHA mock-up, the full MYRRHA mock-up, and the critical core with the ALFRED island. This paper briefly presents the VENUS-F facility, provides a detailed description of the aforementioned critical VENUS-F cores, and compares the numerical results calculated by Serpent to the available experimental data. The compared parameters include keff, point kinetics parameters, fission rate ratios of important actinides to that of U235 (spectral indices), axial and radial distribution of fission rates, and lead void reactivity effect. The reported results show generally good agreement between the calculated and experimental values. Nevertheless, the paper also reveals some noteworthy issues requiring further attention. This includes the systematic overprediction of reactivity and systematic underestimation of the U238 to U235 fission rate ratio.