A chemical approach to the formation of columnar defects involving the growth and incorporation of MgO nanorods into high temperature superconductors (HTS's) has been developed. MgO nanorods were incorporated into Bi2Sr2CaCu2Oz, Bi2Sr2Ca2Cu3Oz, and Tl2Ba2Ca2Cu3Oz superconductors at areal densities up to 2 × 1010/cm2. Microstructural analyses of the composites demonstrate that the MgO nanorods create a columnar defect structure in the HTS matrices, form a compositionally sharp interface with the matrix, and self-organize into orientations perpendicular and parallel to the copper oxide planes. Measurements of the critical current density demonstrate significant enhancements in the MgO nanorod/HTS composites at elevated temperatures and magnetic fields compared with reference samples.