Abstract: Nuclei in the vicinity of 78Ni are important benchmarks for nuclear structure, which can reveal changes in the shell structure far from stability. Spectroscopy of the odd-odd isotope 78Cu was performed for the first time in an experiment with the EURICA setup at the Radioactive Isotope Beam Factory at RIKEN Nishina Center. Excited states in the neutron-rich isotope were populated following the beta decay of 78Ni produced by in-flight fission and and separated by the BigRIPS separator. A level scheme based on the analysis of γ−γ coincidences is presented. Tentative spin and parity assignments were made when possible based on the β-decay feeding intensities and γ-decay properties of the excited states. Time correlations between β and γ decay show clear indications of an isomeric state with a half-life of 3.8(4) ms. Large-scale Monte Carlo shell-model calculations were performed using the A3DA-m interaction and a valence space comprising the full fp shell and the 1g9/2 and 2d5/2 orbitals for both protons and neutrons. The comparison of the experimental results with the shell-model calculations allows interpreting the excited states in terms of spin multiplets arising from the proton-neutron interaction. The results provide further insight into the evolution of the proton single-particle orbitals as a function of neutron number, and quantitative information about the proton-neutron interaction outside the doubly magic 78Ni core.