The use of ultrafast laser pulses is having an impact on materials processing in profound ways. “Machining” with femtosecond pulses affords considerable advantages over nanosecond pulses, such as subdiffraction-limited material ablation, where ablated spot dimensions are below that achievable when longer pulses are focused to the minimum spot size dictated by optical physics. These properties have been exploited to address what had become a critical problem in the semiconductor industry, the repair of patterned photomasks. We will describe how the fundamentals of femtosecond laser ablation have been implemented in a machine designed to repair photomasks. We will also describe experiments designed to deposit Cr metal onto fused-silica substrates using 100-fs, 400-nm light pulses at atmospheric pressure. Multiphoton dissociation of Cr(CO)6 adsorbed on fused-silica substrates initiates Cr deposition. The mechanisms for deposition on both transparent (fused silica) and absorbing (Cr metal) substrates are discussed. Finally, we describe experiments that were carried out to extend the photomask repair process to shorter wavelengths (below 200 nm) using light generated by frequency-mixing of ultrashort, 30-fs pulses in an Ar-filled capillary.