Alumina-based nanocomposites reinforced with niobium and/or carbon nanotubes (CNT) were fabricated by advanced powder processing techniques and consolidated by spark plasma sintering. Raman spectroscopy revealed that single-walled carbon nanotubes (SWCNT) begin to break down at sintering temperatures >1150 °C. Nuclear magnetic resonance showed that, although thermodynamically unlikely, no Al 4C 3 formed in the CNT–alumina nanocomposites, such that the nanocomposite can be considered as purely a physical mixture with no chemical bond formed between the nanotubes and ceramic matrix. In addition, in situ single-edge notched bend tests were conducted on niobium and/or CNT-reinforced alumina nanocomposites to assess their toughness. Despite the absence of subcritical crack growth, average fracture toughness values of 6.1 and 3.3 MPa m 1/2 were measured for 10 vol.% Nb and 10 vol.% Nb–5 vol.% SWCNT–alumina, respectively. Corresponding tests for the alumina nanocomposites containing 5 vol.% SWCNT, 10 vol.% SWCNT, 5 vol.% double-walled-CNT and 10 vol.% Nb yielded average fracture toughnesses of 3.0, 2.8, 3.3 and 4.0 MPa m 1/2, respectively. It appears that the reason for not observing improvement in fracture toughness of CNT-reinforced samples is because of either damage to CNTs or possibly non-optimal interfacial bonding between CNT-alumina.