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Abstract Manufacturing of ceramics is challenging due to their low toughness and high hardness. Additive Manufacturing (AM) has been explored to create complex ceramic structures, but current techniques face a tradeoff between precisely controlled feature sizes and high shrinkage at the microscales. Here, we introduce 3D‐AJP, a novel freeform ceramic fabrication method that enables highly complex microscale 3D ceramic architectures—such as micropillars, spirals, and lattices—with minimal shrinkage and no auxiliary support. Using a near‐binder‐free nanoparticle ink in an Aerosol Jet (AJ) 3D printer, our approach precisely controls feature sizes down to 20 µm with aspect ratios up to 30:1. The resulting structures exhibit exceptionally low linear shrinkage of 2‐6% upon sintering, spanning five orders of magnitude in length scale. Bi‐material 3D architectures (zinc oxide/zirconia, zinc oxide/titania, titania/zirconia) and hybrid ceramics further demonstrate the technique’s versatility. We showcase two key applications. First, 3D ceramic photocatalysts improve water purification performance, achieving a 400% increase in photocatalytic efficiency compared to bulk ceramics. Second, we develop a highly sensitive Her2 biomarker sensor for breast cancer detection, achieving a 22‐second response time and a record‐low detection limit of 0.0193 fm. Our technique will lead to high‐performance sensing, filtration, microelectronics packaging, catalysis, and tissue regeneration technologies.