Poly(glycerol monomethacrylate) (PGMA) prepared by reversible addition−fragmentation chain transfer polymerization was investigated as an additive for high-loading iron oxide nanoparticle (IOP) 3D printable inks. The effect of adjusting the molar mass and loading of PGMA on the rheology of IOP suspensions was investigated, and an optimized ink formulation containing 70% w/w IOPs and 0.25% w/w PGMA 98 at pH 10 was developed. This ink was successfully 3D printed onto various substrates and into several structures, including rectangles, high aspect ratio cylinders, letters, spiral-and comb-shaped structures, and thin-and thick-walled toroids. The effect of sintering on the mechanical properties of printed artifacts was investigated via four-point flexural and compressive testing, with higher sintering temperatures resulting in improved mechanical properties due to changes in the particle size and microstructure. The printed toroids were fabricated into inductors, and their electrical performance was assessed via impedance spectroscopy at a working frequency range of 0.001−13 MHz. There was a clear trade-off between electrical properties and sintering temperature due to a phase change between γ-Fe 2 O 3 and α-Fe 2 O 3 upon heating. Nevertheless, the optimized devices had a Q factor of ∼40 at 10 MHz, representing a superior performance compared to that of other inductors with iron oxide cores previously reported. Thus, this report represents a significant step toward the development of low-cost, fully aqueous, high loading, and 3D printable ceramic inks for high-performance inductors and functional devices.