As the formaldehyde is one of the main indoor pollutants, the purpose of this study is to effectively remove indoor formaldehyde pollution by using environmentally friendly 3D printing ornaments. The wood 3D printing filaments cellulose/polylactic acid composite (Cellu/P) was selected as the starting material, and 3-aminopropyltriethoxysilane (APTES) was used for chemical modification to obtain a series of cellulose composite materials with amino groups. The modified composite materials (APTES@Cellu/P) were characterized by Fourier transform infrared, X-ray diffraction, scanning electron microscope, energy dispersive spectroscopy, thermogravimetric analysis, and mechanical tests, and a formaldehyde removal experiment was performed. The feasibility of 3D printing was evaluated, and the process of 3D printing-functionalized customized ornaments was proposed, and then a school emblem was used for modeling, printing, and surface modification. Compared with the commercially traditional activated carbon, 3D printing-customized ornaments of APTES@Cellu/P material has a better formaldehyde removal effect, and can even avoid the secondary pollution that is common to the activated carbon.