We demonstrate that the energy bandgap of layered, high-dielectric alpha-MoO3 can be reduced to values viable for the fabrication of 2D electronic devices. This is achieved through embedding Coulomb charges within the high dielectric media, advantageously limiting charge scattering. As a result, devices with alpha-MoO3 of similar to 11 nm thickness and carrier mobilities larger than 1100 cm(2) V-1 s(-1) are obtained.