Discovering the effect of magnetic anisotropy on the magnetization configurations of magnetic nanomaterials is essential and significant for not only enriching the fundamental knowledge of magnetics but also facilitating the designs of desired magnetic nanostructures for diverse technological applications, such as data storage devices, spintronic devices, and magnetic nanosensors. Herein, we present a direct observation of magnetocrystalline anisotropy tuning magnetization configurations in uniaxial magnetic nanomaterials with hexagonal structure by means of three modeled samples. The magnetic configuration in polycrystalline BaFe12O19 nanoslice is a curling structure, revealing that the effect of magnetocrystalline anisotropy in uniaxial magnetic nanomaterials can be broken by forming an amorphous structure or polycrystalline structure with tiny grains. Both single crystalline BaFe12O19 nanoslice and individual particles of single-particle-chain BaFe12O19 nanowire appear in a single domain state, revealing a dominant role of magnetocrystalline anisotropy in the magnetization configuration of uniaxial magnetic nanomaterials. These observations are further verified by micromagnetic computational simulations.