A technique to establish electrical contact and perform multi-probe electrical measurements (e.g., four-probe measurements), even at low temperatures, is presented in this work. The natural adhesion contact (NAC) is applicable to the wide range of dimensions of organic crystals. Furthermore, the precise electrode patterns required to carry out multi-probe measurements are guaranteed, in contrast to fine conductive paste painting methods. We demonstrate four-probe electrical measurements of α-(BEDT-TTF)2I3 (where BEDT-TTF = bis(ethylenedithio) tetrathiafulvalene) at temperatures down to 100 K. The obtained temperature dependence showed a steep meta l–insulator transition and exhibited zero hysteresis throughout several measurement sequences.