Electrically conducting zeolite-like frameworks are largely unstudied as electronic materials, but may offer new avenues in energy applications, ranging from electrical energy storage to catalysis. We present two zeolite-like framework materials, a vanadium arsenate [(As 6 V 15 O 51 ) −9 ] ∞ , compound (1), and a vanadium phosphate [(P 6 V 15 O 51 ) −9 ] ∞ , compound (2), their syntheses, and physical and electrical characterization. We compare the electrical characteristics of the two compounds through the measurements of conductivity as a function of temperature and extra-framework constituents. Our results indicate that compound (1) is a mixed conductor with framework electronic conduction and ionic conduction associated with the extra-framework constituents. Compound (2), in contrast, shows only ionic conductivity. Probing the electronic properties of zeolite-like mixed conductors paves the way for the innovative use of these materials.