The high-pressure structure and dynamics of PbZr0.40Ti0.60O3 were investigated by means of neutron diffraction, X-ray diffraction, and resonance Raman spectroscopy. The complex (P4mm, Cm, Cc, F1, F (1) over bar) phase transition sequence is characterized by these techniques. On the basis of the results of structure refinements, the high-pressure behavior of the spontaneous polarization, the (Zr,Ti)O-6 rotation angles, and the polarization rotation angle are obtained. Moreover, resonance Raman spectra combined with previous Raman data in the literature provide evidence that the pressure-induced transition to the monoclinic Cm space group and the above transition sequence terminating in a paraelectric state are general features of Pb(Zr1-xTix)O-3 (0.48 <= x <= 1).