Simultaneous [18 F]-fluorodeoxyglucose positron emission tomography and functional magnetic resonance imaging (FDG-PET/fMRI) provides the capability to image two sources of energetic dynamics in the brain – cerebral glucose uptake and the cerebrovascular haemodynamic response. Resting-state fMRI connectivity has been enormously useful for characterising interactions between distributed brain regions in humans. Metabolic connectivity has recently emerged as a complementary measure to investigate brain network dynamics. Functional PET (fPET) is a new approach for measuring FDG uptake with high temporal resolution and has recently shown promise for assessing the dynamics of neural metabolism. Simultaneous fMRI/fPET is a relatively new hybrid imaging modality, with only a few biomedical imaging research facilities able to acquire FDG PET and BOLD fMRI data simultaneously. We present data for n = 27 healthy young adults (18–20 yrs) who underwent a 95-min simultaneous fMRI/fPET scan while resting with their eyes open. This dataset provides significant re-use value to understand the neural dynamics of glucose metabolism and the haemodynamic response, the synchrony, and interaction between these measures, and the development of new single- and multi-modality image preparation and analysis procedures.