Synthetic MRI using a multi-delay multi-echo sequence was applied to a pre-term neonatal and full term neonatal population. The brain was segmented into different tissue types using the relaxometric data and using an improved algorithm which suppresses CSF partial volume fractions in grey matter. The volumes and volume fractions were calculated. The relation between volumetric quantities and either gestational age (preterm patients only), or corrected age (whole population) was investigated. The Brain Parenchymal and grey matter fraction were found to be dependent on gestational age at birth, while grey matter, CSF, intracranial and brain parenchymal volume are dependent on age.