Engineering ceramics have high stiffness, excellent thermostability, and relatively low density, but their brittleness impedes their use as structural materials. Incorporating carbon nanotubes (CNTs) into a brittle ceramic might be expected to provide CNT/ceramic composites with both high toughness and high temperature stability. Until now, however, materials fabrication difficulties have limited research on CNT/ceramic composites. The mechanical failure of CNT/ceramic composites reported previously is primarily attributed to poor CNT–matrix connectivity and severe phase segregation. Here we show that a novel processing approach based on the precursor method can diminish the phase segregation of multi-walled carbon nanotubes (MWCNTs), and render MWCNT/alumina composites highly homogeneous. The MWCNTs used in this study are modified with an acid treatment. Combined with a mechanical interlock induced by the chemically modified MWCNTs, this approach leads to improved mechanical properties. Mechanical measurements reveal that only 0.9 vol% acid-treated MWCNT addition results in 27% and 25% simultaneous increases in bending strength (689.6 ± 29.1 MPa) and fracture toughness (5.90 ± 0.27 MPa m^1/2), respectively.