This dataset contains scanning electron diffraction (SED) data used in the publication entitled "Microstructural and mechanical characterisation of a second generation hybrid metal extrusion & bonding aluminium-steel butt joint". The data denoted “SED_HYB_...” were recorded from an aluminium-steel interface region that includes aluminium and steel grains, an interfacial Al-Fe-Si layer, and dispersoids and some oxide particles located within the aluminium region. The nanoscale interfacial intermetallic phase layer is polycrystalline, and to increase the probability of recording data from intermetallic phase crystals oriented close to zone axes, the data were recorded in a tilt series covering 30 degrees, in steps of 1 degree. The file names give the goniometer x-tilt values in degrees, e.g. " SED_HYB_TX-150.hdf5" denotes an x-tilt of -15.0 degrees. SED data recorded from an Au cross-grating specimen, named "SED_AuX.hdf5", and from a MoO3 specimen, named "SED_MoO3.hdf5", are also included for calibration purposes.