Here, we report an air-free approach to infiltrate isostructural metal-organic frameworks (MOFs), M-MOF-74 (M = Cu, Mn, Zn, Mg), with conjugated acceptor 7,7,8,8-tetracyanoquinodimethane (TCNQ). The TCNQ@M-MOF-74 compounds exhibit a striking correlation between their bulk conductivities and the open d shell variants (Cu, Mn), arising from TCNQ p-doping of the MOFs. Importantly, conjugation of the guest molecule is a prerequisite for inducing electrical conductivity in these systems. Here, we report an air-free approach to infiltrate isostructural metal-organic frameworks (MOFs), M-MOF-74 (M = Cu, Mn, Zn, Mg), with conjugated acceptor 7,7,8,8-tetracyanoquinodimethane (TCNQ).