AbstractIn recent years, photopolymerization has been found wide applications in industry and daily life, while many defective properties of polymers limit their development, including compressive strength, mechanical properties, and functions. Furthermore, zeolites are microporous solids with many industrial applications. As fillers they can improve mechanical properties of zeolite/polymer composite and transfer their properties to composites. Here the fabrication is reported of composites with very high filler contents (80–95 wt%) under mild photopolymerization conditions (visible LED light irradiation, room temperature, under air). Compared to pure poly(ethylene glycol) diacrylate (PEGDA) polymer, mechanical properties have been greatly improved, and the storage modulus increased by nearly 20‐fold compared to that of pure polymer. After debinding/sintering of composites by high temperature treatment, zeolite porosity is preserved with good adsorption capacities. Some step‐like object with 3D structure is also obtained by an original 3D printing technique noted “layer by layer molding/curing.” Hence, as a great breakthrough, this work is expected to lead to a valuable development in the field of photopolymerization in quite highly filled composites. This also will expand their potential applications for 3D printing in the fields of high‐performance lightweight materials and adsorption, and opens the door to a new process of zeolite shaping.