A method to produce highly efficient and long-range vertical charge transport is demonstrated in an undoped polythiophene thin film, with average mobilities above 3.1 cm(2) V-1 s(-1). These record high mobilities are achieved by controlled orientation of the polymer crystallites enabling the most efficient and fastest charge transport along the chain backbones and across multiple chains. The significant increase in mobility shown here may present a new route to producing faster and more efficient optoelectronic devices based on organic materials. [GRAPHICS] .