jats:pThe ability of quantum computers to overcome the exponential memory scaling of many-body problems is expected to transform quantum chemistry. Quantum algorithms require accurate representations of electronic states on a quantum device, but current approximations struggle to combine chemical accuracy and gate efficiency while preserving physical symmetries, and rely on measurement-intensive adaptive methods that tailor the wave function to each molecule. In this contribution, we present a symmetry-preserving and gate-efficient that provides chemically accurate molecular energies with a well-defined circuit structure. Our approach exploits local qubit connectivity, orbital optimization, and connections with generalized valence bond theory to maximize the accuracy that is obtained with shallow quantum circuits. Numerical simulations for molecules with weak and strong electron correlation, including benzene, water, and the singlet-triplet gap in tetramethyleneethane, demonstrate that chemically accurate energies are achieved with as much as 84% fewer two-qubit gates compared to state-of-the-art adaptive techniques.</jats:p> jats:sec jats:title/ jats:supplementary-material jats:permissions jats:copyright-statementPublished by the American Physical Society</jats:copyright-statement> jats:copyright-year2024</jats:copyright-year> </jats:permissions> </jats:supplementary-material> </jats:sec>