Abstract: Micromorphologically crack-free vitreous carbon articles having a length and width each of which is at least 10 mm, and a thickness of at least 5 mm are described, as well as multilayer laminates of micromorphologically crack-free vitreous carbon, and corresponding methods and apparatus for manufacture of same. 3D printed vitreous carbon articles are also described, together with 3D printing apparatus and methods for producing same. Methods are also described for forming vitreous carbon containing vitreous carbon nanolattice articles therein as filler. The vitreous carbon compositions, articles, and laminates of the disclosure overcome the thickness limitations of conventional vitreous carbon manufacturing methods and the microcracking issues attendant previous efforts to produce vitreous carbon of substantial size and thickness.