Samples of cobalt-doped neodymium orthoferrite compounds, NdCo
x
Fe
1−x
O
3
(0.0 ≤ x ≤ 0.5) were synthesized via glycine auto-combustion between 250 and 300°C and calcined at 500°C for 2 h. X-ray diffraction showed that all compounds had an orthorhombic perovskite structure with space group Pbnm. Increasing cobalt doping gradually reduced the lattice parameters and contracted the unit cell volume. Both X-ray diffraction and scanning electron microscopy showed that the particles were spherical and in the nano-sized range (19–52 nm) with pores between grains. Vibrating sample magnetometry at room temperature indicated that NdFeO
3
has a high coercive field (1950 Oe) and cobalt substitution for iron led to a decrease in the coercive field, saturation and remanent magnetization, which was as a result of decreased magnetic moments in the crystal and reduced canting of the FeO
6
octahedra. The increase in magnetization and coercive fields with increase of Co was connected to the microstructure (bond lengths and angles, defects, pores, grain boundaries) and crystallite size. The compounds NdCo
x
Fe
1−x
O
3
show antiferromagnetism with weak ferromagnetism due to uncompensated non-collinear moments. These compounds could serve as prototypes for tuning the properties of magnetic materials (ferromagnetic and antiferromagnetic) with potential applications in data storage, logic gates, switches and sensors.