In the present paper, high pressure data from a synchrotron X-ray diffraction study on a lillianite (Pb3Bi2S6) single crystal up to approximately 21 GPa are presented.A phase transition from lillianite (Bbmm space group #63, LP lillianite) to the high-pressure form β-Pb3Bi2S6 (Pbnm space group, HP lillianite) was confirmed and bracketed between 4.90 and 4.92 GPa.The transition is reversible but of first-order with a hysteresis of ~2.8 GPa. The phase transition to β-Pb3Bi2S6 showed weak effects of pseudomerohedral twinning that disappeared upon decompression, testifying to a full recovery of the single crystal of lillianite. This makes lillianite an interesting shapememory material.With a bulk modulus K4.9 = 78(3) GPa and K' = 5.1(4), β-Pb3Bi2S6 is markedly less compressibile than lillianite [K0 = 44(2) GPa, K' = 7( 1)]. Compressional anisotropy increased markedly in β-Pb3Bi2S6 with compressibility along the b axis [M0b = 130(6) GPa and M'b = 19(3) in lillianite, M4.9b = 145( 4) GPa and This is the peer-reviewed, final accepted version for American Mineralogist, published by the Mineralogical Society of America.The published version is subject to change. Cite as Authors (Year) Title. American Mineralogist, in press.