Recent years have seen an increased application of small-scale uniaxial testing—microcompression—to the study of plasticity in macroscopically brittle materials. By suppressing fast fracture, new insights into deformation mechanisms of more complex crystals have become available, which had previously been out of reach of experiments. Structurally complex intermetallics, metallic compounds, or oxides are commonly brittle, but in some cases extraordinary, though currently mostly unpredictable, mechanical properties are found. This paper aims to give a survey of current advances, outstanding challenges, and practical considerations in testing such hard, brittle, and anisotropic crystals.