This study examines the deformation response of 20, 5, and 1 micron diameter samples fabricated by FIB-milling from bulk ultrapure LiF single crystals. The bulk crystals have a very low initial dislocation density as revealed by an etch-pit technique. Two types of <001> microsamples were deformed preferentially by single slip when compressed inside a nanoindentation system. Similar to previously studied FCC-derivative metals, LiF microsamples demonstrate dramatic strengthening achieving the engineering flow stress σ ≈ 650 MPa in 1-μm samples. The stress-diameter dependence obeys a power law, σ ∼ D−m
, where m ≈ 0.8. Stochastic variation of flow stress, fast intermittent deformation events (“avalanches”) and highly localized slip bands after avalanches - all characteristic of size effects in metals, are also observed in LiF. Possible dislocation mechanisms of the observed size effects are discussed.