We explore the response of Ir 5d orbitals to pressure in β-Li2IrO3, a hyperhoneycomb iridate in proximity to a Kitaev quantum spin liquid (QSL) ground state. X-ray absorption spectroscopy reveals a reconstruction of the electronic ground state below 2 GPa, the same pressure range where x-ray magnetic circular dichroism shows an apparent collapse of magnetic order. The electronic reconstruction, which manifests a reduction in the effective spin-orbit (SO) interaction in 5d orbitals, pushes β-Li2IrO3 further away from the pure J eff = 1/2 limit. Although lattice symmetry is preserved across the electronic transition, x-ray diffraction shows a highly anisotropic compression of the hyperhoneycomb lattice which affects the balance of bond-directional Ir-Ir exchange interactions driven by spin-orbit coupling at Ir sites. An enhancement of symmetric anisotropic exchange over Kitaev and Heisenberg exchange interactions seen in theoretical calculations that use precisely this anisotropic Ir-Ir bond compression provides one possible route to realization of a QSL state in this hyperhoneycomb iridate at high pressures.The novel electronic ground states of 5d-based compounds driven by spin-orbit interactions continue to provide an excellent playground for the realization of unconventional quantum phases of matter including topological insulators [1-4] and quantum spin-liquids (QSLs) [5][6][7]. One example of the latter is the non-trivial QSL ground state of the Kitaev model [8], a rare example of a solvable interacting quantum model with Majorana fermions as its elementary excitations. Material candidates for possible realization of the Kitaev model include honeycomb-based-lattice systems with strong spin-orbit coupling [6,9], such as the two and three-dimensional honeycomb iridates, α-Li(Na) [7,[20][21][22] as well as α-RuCl 3 [23,24]. However, it is experimentally established that these materials order magnetically at low temperatures [17,18,20,[25][26][27], spoiling numerous attempts to realize the Kitaev QSL. Hence, tuning structure and related intricate interactions present in these materials through chemical or physical pressure provides a potential route to introduce magnetic frustration and realize novel phases of matter.In this Letter we have investigated the electronic and structural response of β-Li 2 IrO 3 to high pressure. Xray absorption near edge structure (XANES) measurements at Ir L-edges reveal a dramatic suppression of the isotropic Ir (L 3 /L 2 ) branching ratio at P ∼ 1.5 GPa, signaling a reduction in the effective strength of spinorbit interactions in the 5d band. This is the same pressure at which net magnetization in applied field collapses [17]. The reconstructed electronic state preserves the L z / S z orbital-to-spin moment ratio of Ir magnetic moments and the insulating ground state indicating that spin-orbit interactions and Mott physics con-