Small‐scale, intensified chemical reactors (i.e., process intensification) mediated by structured catalysts substantially diminishes the advantages of large‐scale gas‐to‐liquid (transport fuels) process plants and can be realized at low capital costs, minimum energy consumption, and zero/small CO2 footprints. Current structured‐catalysts approaches are complex and expensive; therefore, simple methods are crucial that are capable of depositing a desired geometry of catalysts into engineered channels. Herein, we developed printable composition by incorporating nickel and molybdenum ions into water‐soluble PVA and starch; the subsequent pyrolysis of organic compounds resulted into three‐dimensional carbon scaffold with micro/macro interconnected pores (dpore, 6.5 Å; dpore, 100 μm) containing up to 25 wt % catalyst loading. 2 D (TEM, SEM) and 3D (X‐ray computed tomography) microstructural analyses and catalytic tests (conversion of syngas to alcohols) were performed for 3 D printed catalysts and compared with conventional pelleted catalysts. At a high feed flow rate (6000 h−1), CO conversion is rapidly reduced to 16 mol % for pelleted catalysts, whereas 3 D printed catalysts converted 35 mol % of CO, with the same catalyst loading.