Printing ceramic/metal parts increases the number of applications in additive manufacturing technology, but printing different materials on the same object with different mechanical properties will increase the difficulty of printing. Multi-material additive manufacturing technology is a solution. This study develops a novel tape-casting 3D printing technology that uses bottom-up photopolymerization to fabricate the green body for low-temperature co-fired ceramics (LTCC) that consist of ceramic and copper. The composition of ceramic and copper slurries is optimized to allow printing without delamination and sintering without cracks. Unlike traditional tape-casting processing, the proposed method deposits two slurries on demand on a transparent film, scrapes it flat, then photopolymerization is induced using a liquid crystal displayer to project the layer pattern beneath the film. The experimental results show that both slurries have good bonding strength, with a weight ratio of powder to resin of 70:30, and print a U-shaped copper volume as a circuit within the LTCC green body. A three-stage sintering parameter is derived using thermogravimetric analysis to ensure good mechanical properties for the sintered part. The SEM images show that the ceramic/copper interface of the LTCC sintered part is well-bonded. The average hardness and flexural strength of the sintered ceramic are 537.1 HV and 126.61 MPa, respectively. Volume shrinkage for the LTCC slurry is 67.97%, which is comparable to the value for a copper slurry of 68.85%. The electrical resistance of the printed copper circuit is 0.175 Ω, which is slightly greater than the theoretical value, hence it has good electrical conductivity. The proposed tape-casting 3D printer is used to print an LTCC benchmark. The sintered benchmark part is validated for the application in the LTCC application.