Disordered carbon materials, both amorphous and with long-range order, have been used in a variety of applications, from conductive additives and contact materials to transistors and photovoltaics. Here we show a flexible solution-based method of preparing thin films with tunable electrical properties from suspensions of ball-milled coals following centrifugation. The as-prepared films retain the rich carbon chemistry of the starting coals with conductivities ranging over orders of magnitude, and thermal treatment of the resulting films further tunes the electrical conductivity in excess of 7 orders of magnitude. Optical absorption measurements demonstrate tunable optical gaps from 0 to 1.8 eV. Through low-temperature conductivity measurements and Raman spectroscopy, we demonstrate that variable range hopping controls the electrical properties in as-prepared and thermally treated films and that annealing increases the sp 2 content, localization length, and disorder. The measured hopping energies demonstrate electronic properties similar to amorphous carbon materials and reduced graphene oxide. Finally, Joule heating devices were fabricated from coal-based films, and temperatures as high as 285°C with excellent stability were achieved. KEYWORDS: Coal, amorphous carbon, organic semiconductors, thin films, solution processing C arbon has long been known as one of the most chemically versatile elements. As a result, carbonaceous materials have been of technological interest for their wide range of electronic propertiesresulting in materials ranging from low cost conducting materials such as graphite and carbon black, to semiconducting fullerenes and carbon nanotubes, and to insulating diamond and diamond-like carbon. Specifically, carbon black, carbon filaments, and other carbon materials are used in electrodes, conductivity additives, and electromagnetic reflectors. 1 Graphitic materials 2 and amorphous carbon (a-C) 3,4 are the leading and a promising candidate, respectively, for anode materials in lithium ion batteries. Amorphous carbon has also been used in the manufacturing of transistors 5,6 and photovoltaic devices, 7,8 and nanostructured graphitic materials (such as graphene and reduced graphene oxide) have gained significant attention for applications including in photovoltaics, 9−11 transparent conductive membranes, 12−16 and Joule heating devices. 17−19 Despite decades of research on synthetically processed carbon materials, facile, tunable, 20 low-temperature, solution processing methods remain elusive. Carbon black synthesis requires temperatures as high as 2000°C, 21 and a-C is typically deposited by plasma-enhanced chemical vapor deposition (CVD) 22,23 although aerosol-assisted CVD has recently been demonstrated. 8 While extensive research has been conducted to develop solution-based methods of graphene deposition, rGO films remain several orders of magnitude less conductive than CVD graphene. 16,24,25 In contrast to the widely studied world of synthetic carbonaceous materials, the optical...