Abstract: Hexagonal LuFe2O4 is a promising charge order (CO) driven multiferroic material with high charge and spin-ordering temperatures The coexisting charge and spin orders on Fe3+/Fe2+ sites result in magnetoelec. behaviors, but the coupling mechanism between the charge and spin orders remains elusive. Here, by tuning external pressure, we reveal three charge-ordered phases with suggested correlation to magnetic orders in LuFe2O4: (i) a centrosym. incommensurate three-dimensional CO with ferrimagnetism, (ii) a non-centrosym. incommensurate quasi-two-dimensional CO with ferrimagnetism, and (iii) a centrosym. commensurate CO with antiferromagnetism. Exptl. in situ single-crystal X-ray diffraction and X-ray magnetic CD measurements combined with d. functional theory calculations suggest that the charge d. redistribution caused by pressure-induced compression in the frustrated double-layer [Fe2O4] cluster is responsible for the correlated spin-charge phase transitions. The pressure-enhanced effective Coulomb interactions among Fe-Fe bonds drive the frustrated (1/3, 1/3) CO to a less frustrated (1/4, 1/4) CO, which induces the ferrimagnetic to antiferromagnetic transition. Our results not only elucidate the coupling mechanism among charge, spin, and lattice degrees of freedom in LuFe2O4, but also provide a new way to tune the spin-charge orders in a highly controlled manner.