Diffractive optics fabrication is performed by two complementary processing methods that rely on the photoablation of materials by ultrashort UV laser pulses. The spatially selective ablation of materials permits the direct microetching of high-quality surface-relief patterns. In addition, the direct, spatially selective transfer of the ablated material onto planar and nonplanar receiving substrates provides a complementary microprinting operation. The radiation from the ultrashort pulsed excimer laser results in superior quality at relatively low-energy density levels, owing to the short absorption length and minimal thermal-diffusion effects. Computer-generated holographic structures are produced by both modes of operation. Submicrometer features, including Bragg-type structures, are microprinted onto planar and high-curvature optical-fiber surfaces, demonstrating the unique ability of the schemes for complex microstructure and potentially nanostructure development.