This study aimed to map the acute effects of caffeine ingestion on the rate of oxygen metabolosm and blood flow across cerebtal grey matter with a novel MRI method. Sixteen healthy caffeine consumers (8 male, 8 female; age = 24.7 5.1) were recruited to this randomised, double-blind, placebo-controlled drug study. Each participant was scanned on two separate days before and after the delivery of an oral caffeine (250mg) or placebo capsule. The data associated with this project is the original data used for the analysis, mainly composed by NIfTI and text files. A first set of measurements was obtained by applying a newly proposed estimation approach applied to data from an fMRI experiment employing a dual calibration approach that uses hypercapnia and hyperoxia to modulate brain blood flow and oxygenation. Estimates were based on a forward model that describes analytically the contributions of BOLD, cerebral blood flow (CBF) and of the measured end-tidal partial pressures of CO2 and O2 to the acquired dual echo GRE signal. The method allows the estimate of grey matter maps of: oxygen extraction fraction (OEF), CBF, CBF-related cerebrovascular reactivity (CVR), venous cerebral blood volume (CBV) and cerebral metabolic rate of oxygen consumption (CMRO2). A second set of measurements obtained with this data includes estimates of CBF and tissue arrival time (TAT) obtained with an already validated multi inversion time ASL technique (mTI-ASL). Finally we report salivary samples of the caffeine concentration and behavioural data looking at the effects of caffeine on mood and physical sensations.