Pressure-induced structural transformations in relaxor-based perovskite-type (ABO3) 0.9PbZn1/3Nb2/3O3-0.1PbTiO3 single crystals which have a very high piezoelectric response were studied by single-crystal x-ray diffraction and Raman spectroscopy at room temperature and pressures up to 18.1 GPa. Changes in the state of long-range order were observed near 1.0, 2.1, and 5.9 GPa. Initially, upon pressure increase, the ferroic deviation of the atomic positions from the cubic structure is reduced, but the ferroelectric twinning is enhanced, and near 1.0 GPa, the intrinsic ferroelectric multiphase domain pattern formed in the as-synthesized crystals is changed. At 2.1 GPa, the system undergoes a phase transition from a ferroelectric to a relaxor state, which exhibits an average cubic structure but still contains polar nanoregions. At 5.9 GPa, a reversible phase transition typical of Pb-based perovskite-type relaxors occurs, namely a cubic-to-antiferrodistortive phase transition resulting in a long-range order of antiphase octahedral tilts. On decompression, the ferroelectric state reappears below 2.1 GPa, and the local atomic structure is fully recovered at ambient pressure, but the final domain texture differs from the initial one. Ruthenium doping on the B site does not influence the pressure-induced structural transformations.