wileyonlinelibrary.com(OSCs) and organic fi eld-effect transistors (OFETs) and have rather rough surfaces with grain structures, possess relatively large macroscopic gaps between grains and other grains, substrates, or electrodes. [ 3,4 ] Densities of vacuum-deposited and solution-processed organic fi lms are generally lower than those of single crystals. [ 5 ] The typical difference in density between organic fi lms and single crystals is several to over ten percent, which corresponds to the total volume of gaps in an organic fi lm. Such gaps in amorphous and polycrystalline fi lms might be expected to impede carrier injection and transport because of ineffi cient carrier movement through indirect routes to avoid the gaps. For example, carrier movement across gaps between grains is a limiting step because they might be potential barriers or carrier traps. [ 6,7 ] The removal of gaps between grains enhanced carrier mobilities in OFETs containing polycrystalline organic fi lms. [ 8,9 ] Densities of amorphous organic fi lms depend on substrate temperature during vacuum deposition, with density variation of around 1%. For example, fi lms of stable organic glasses with high densities form at T substrate / T g = 0.8−0.9, where T substrate is the substrate temperature during vacuum deposition and T g is the glass transition temperature of an organic material. [ 10 ] Lower water uptake was realized in denser organic fi lms vacuum deposited at a suitable substrate temperature. [ 11 ] Low water uptake should improve the long-term air stability of organic devices because water promotes the degradation of organic materials, especially in the presence of photo generated excited states and redox-generated radicals, cations, and anions. [ 12,13 ] We expect that the electrical characteristics and air stability of organic devices, such as OLEDs, OSCs, and OFETs, will be enhanced if the macroscopic and microscopic gaps in the organic fi lms are removed.Our strategy to remove the gaps from organic fi lms is very simple: the gaps are irreversibly compressed by applying high pressure to polycrystalline and amorphous organic fi lms. To compress the fi lms, we focused our attention on cold isostatic pressing (CIP) and hot isostatic pressing (HIP). CIP and HIP have been widely used to compress and mold metal, ceramic, plastic, and composite powders into certain forms. [14][15][16] In this approach, the powder is enclosed in a fl exible, sealed rubber bag and immersed in a pressurization vessel fi lled with a liquid. Standard metal mold pressing (MMP) applies uniaxial The spatial gaps in organic fi lms 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 fi lms by ineffi cient molecular packing are diffi cult to compress using CIP and HIP; however, the macroscopic gaps formed between grains and other grains or substrates in polycrystalline organic fi lms can be compressed using CIP and HIP. The gap com...