Infants born preterm are at risk of neurodevelopmental delays in childhood, and MRI may improve knowledge of underlying cerebral changes. Relationships were investigated between whole brain volumes and microstructure in 256 preterm infants and neurodevelopmental outcomes at age 2 years using voxel-based morphometry and tract-based spatial statistics. Lower grey and white matter volumes and altered white matter microstructure were associated with poorer outcomes. In general, relatively widespread brain regions were associated with cognition, more central regions with cerebral palsy, and more peripheral regions with language. This study provides further understanding of how brain structure in preterm infants is related to longer-term outcomes.