Grain-oriented ferroelectric ceramics are desirable for many applications, but developing a mass-production method for such kinds of ceramics remains a significant challenge. In the current study, we report a convenient approach combining magnetic alignment and gelcasting to prepare grain-oriented ceramics without applied pressure and templates. This method was found to be effective to prepare highly a-b plane-oriented Bi4Ti3O12 ferroelectric ceramics and subsequently enhance the dielectric properties. We used the conventional ceramic process, i.e., solid-state synthesis, gelcasting forming technique, and pressureless sintering except for the application of a 10 T magnetic field. Indeed, such an approach should facilitate the mass production of large and dense grain-oriented ceramic materials.