The results are reported of the pressure (P) dependence of the electrical resistance (R), the thermoelectric power (Seebeck effect) (S), and compressibility as well as the time dependence of R at fixed P up to 20 GPa for four metallo-organics based on the BEDT-TTF (bisethylenedithiolo-tetrathiofulvalene) group, theta-(BEDT-TTF)(2)CsZn(SCN)(4), alpha-(BEDT-TTF)(2)I-3, beta'-(BEDT-TTF)(2)PF6, and (BEDT-TTF)-TCNQ. X-ray powder and single-crystal diffraction studies were also made on theta-(BEDT-TTF)(2)CsZn(SCN)(4) at high pressures up to P similar to 10 GPa. The R values of all the crystals decreased with pressure up to P similar to 3-5 GPa (low-pressure regime), and then the sign of dR/dP inverted (high-pressure regime). From the investigation of the mechanical and structural properties, these materials were found to have a large compressibility in the low-pressure regime, and a small one in the high-pressure region. In theta-(BEDT-TTF)(2)CsZn(SCN)(4) we observed pressure-induced reversible degradation (amorphization) in structure without a solid-phase reaction. (C) 2007 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.