A novel brain segmentation method, based on quantitative R1, R2 and PD maps measured using a multi-delay multi-echo sequence, was tested on very preterm neonates. The intracranial, brain and CSF volumes and fractions were determined using both the quantitative method and MANTiS, an established atlas-based segmentation method. The results of both methods were compared by using Bland-Altman plots and by quantifying the overlap by co-registering the different segment maps and calculating the Dice score. Despite some systematic differences in the volumetric results, both methods agree well. This study shows that segmentation using quantitative data functions well even for neonates.