focused on research and product development of carbon-based materials, exemplified by the discoveries of fullerene, [10] carbon nanotubes [11] and graphene, [12] as well as fabrication of porous carbon [13] and carbon black additives for many commercial applications. [14] However, most industries can only employ these functional carbon materials as fillers, necessitating additional components, often polymer matrices, for imparting processability. [15,16] The presence of matrix materials can greatly diminish many intrinsic advantages of carbons, leading to compromised material performance. Furthermore, necessary steps of mixing and processing in composite manufacturing may lead to high energy consumption and carbon footprint, resulting in an enormous negative impact on the environment. Enabling ondemand manufacturing of carbons with controlled macroscopic structures is necessary to unlock their full potential in various applications, while addressing urgent societal challenges including climate change and environmental sustainability.Generally, creating structured carbon materials rely on the use of polymer precursors, combined with pyrolysis-based approaches to allow their conversion to carbon materials. [17][18][19] A common example in this area is carbon fiber manufacturing, which uses polyacrylonitrile (PAN) as a carbon precursor and involves multiple processing steps, including fiber spinning, drawing, thermal stabilization/crosslinking and carbonization. [20] Alternatively, many other carbon precursors have been reported, including pitch-based chemicals, [21] lignin, [22,23] cellulose, [24,25] polyethylene (PE), [26][27][28] polypropylene (PP) [29,30] and polybenzoxazines. [31,32] While these chemical can be effectively converted to carbons, the scope of most work in the area of structured carbon production is associated with fibril materials; [33] the ability of manufacturing carbon with complex architectures at macroscopic scale is largely underexplored.In recent years, additive manufacturing (AM) has attracted significant attention in both academic research labs and largescale manufacturing facilities, leading to wide recognition as a key future manufacturing technology. [34] AM can create products through layer-by-layer addition without the need for tools and molds, which is also inherently less wasteful than traditional subtractive-based methods due to its significantly Carbon materials are essential to the development of modern society with indispensable use in various applications, such as energy storage and high-performance composites. Despite great progress, on-demand carbon manufacturing with control over 3D macroscopic configuration is still an intractable challenge, hindering their direct use in many areas requiring structured materials and products. This work introduces a simple and scalable method to generate complex, large-scale carbon structures using easily accessible materials and technologies. 3D-printed, commercial polypropylene (PP) parts can be thermally stabilized through cracking-faci...