The brittle-to-ductile transition (BDT) has been established for NiAl single crystals as evaluated by fracture toughness testing and also the effects of prestraining on the brittle-to-ductile transition temperature (BDTT) have been investigated. Specimens were prestrained to a 10% plastic strain level at 200°C under tension prior to toughness testing. The BDT of the prestrained specimens was compared to that of the as homogenized specimens. The results have revealed the occurrence of two competing effects upon prestraining: (1) an increase in dislocation sources causing a difficulty in micro-crack initiation and resulting in an increase in toughness at low temperatures, and (2) an increase in the flow stress resulting in an increase in BDT temperature. The crack initiation and propagation mechanisms were also analyzed and have been discussed.