The spatial gaps in organic films are compressed using cold and hot isostatic pressing (CIP and HIP, respectively) with the aim of enhancing their electrical characteristics. The microscopic gaps formed in amorphous organic films by inefficient molecular packing are difficult to compress using CIP and HIP; however, the macroscopic gaps formed between grains and other grains or substrates in polycrystalline organic films can be compressed using CIP and HIP. The gap compression by CIP and HIP in polycrystalline films enhances their electrical characteristics. Conversely, the electrical characteristics of amorphous films remain unchanged after CIP and HIP. HIP gives almost the same results as CIP in terms of gap compression and current enhancement, probably because the expected activation of molecular motion at high temperature is suppressed under high applied pressure. CIP markedly improves the performance of organic light-emitting diodes, organic solar cells, and organic field-effect transistors containing polycrystalline films. These findings are important for understanding the carrier injection and transport mechanisms of organic films containing gaps as well as enhancing the performance of future organic devices, especially those with polycrystalline films.