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Although intermetallics are attractive for their high strength, many of them are often brittle at room temperature, thereby severely limiting their potential as structural materials. Here, we report on a previously unidentified deformable nanocrystalline CoAl intermetallics with Co-rich thick grain boundaries (GBs). In situ micropillar compression studies show that nanocrystalline CoAl with thick GBs exhibits ultrahigh yield strength, exceeding 4.5 gigapascals. Unexpectedly, nanocrystalline CoAl intermetallics also show prominent work hardening to a flow st