© 2025 authors. Published by the American Physical Society. Published by the American Physical Society under the terms of the ''https://creativecommons.org/licenses/by/4.0/''Creative Commons Attribution 4.0 International license. Further distribution of this work must maintain attribution to the author(s) and the published article's title, journal citation, and DOI. Open access publication funded by CERN.Shape coexistence, a collective manifestation of nuclear structure, emerges from the underlying single-particle dynamics and is prominently observed in the region below Ni68. Theoretical studies have emphasized the key role of the ?d5/2 orbital, the quadrupole partner of ?g9/2, in driving deformation. However, experimental constraints on the location and properties of neutron orbitals in neutron-rich isotopes in this region remain scarce. In this Letter, the single-particle structure of Ni69 was investigated via the Ni68(d,p) reaction in inverse kinematics, performed at the ISOLDE Solenoidal Spectrometer at CERN. Several new excited states were observed, and comparisons with adiabatic distorted wave approximation (ADWA) calculations enabled ?-value assignments for the most strongly populated states. In particular, a state at 2.56 MeV is interpreted as the dominant fragment of the ?d5/2 strength. The experimental findings are well reproduced by Large-Scale Shell Model calculations using a modified LNPS interaction with an increased ?g9/2-?d5/2 energy gap. These results provide new insight into the structure of Ni69 and underscore the crucial role of the ?d5/2 orbital in the onset of collectivity at the N=40 island of inversion.