The level structure of 36Al has been studied via β decay of 36Mg at the Facility for Rare Isotope Beams (FRIB) and the National Superconducting Cyclotron Laboratory (NSCL). A long-lived isomer in 36Al was identified which decays by β to an excited state of 36Si. The ground state and the isomeric state of 36Al were found to populate different energy levels of 36Si. The results from the two data sets in the present work complement each other. Configuration interaction calculations performed with the FSU shell-model Hamiltonians provide reasonable descriptions to the experimental observations and offer insight into future improvements of the theoretical interpretation.