This paper presents all-dielectric materials used to 3D print coupons with spatially varying dielectric permittivity and possessing high dielectric anisotropy. The coupons were directly printed through a dual-filament fused deposition modelling technique utilizing bespoke feedstock filament comprised a polymer-based micro-ceramic composite with controlled permittivity and loss. By designing the arrangement of both high and low permittivity filament materials in the printed coupons, the microwave operating frequency and magnitude of Mie-type resonances could be manipulated to provide metamaterial-like characteristics.