Anisotropy is an important and widely present characteristic of materials that provides desired direction-dependent properties. In particular, the introduction of anisotropy into magnetic nanoparticles (MNPs) has become an effective method to obtain new characteristics and functions that are critical for many applications. In this review, we first discuss anisotropy-dependent ferromagnetic properties, ranging from intrinsic magnetocrystalline anisotropy to extrinsic shape and surface anisotropy, and their effects on the magnetic properties. We further summarize the syntheses of monodisperse MNPs with the desired control over the NP dimensions, shapes, compositions, and structures. These controlled syntheses of MNPs allow their magnetism to be finely tuned for many applications. We discuss the potential applications of these MNPs in biomedicine, magnetic recording, magnetotransport, permanent magnets, and catalysis. CONTENTS 4.5.1. Co-Based Rare-Earth Metal Alloy Nanoparticles 3917 4.5.2. Fe-Based Rare-Earth Metal Alloy Nanoparticles 4.6. Rare-Earth-Metal-Free Nanoparticles 4.6.1. MnBi and MnAl Nanoparticles 4.6.2. Metal Carbide Nanoparticles 5. Magnetic Nanoparticles with Enhanced Anisotropy for Biomedical Applications 5.1. Magnetic Nanoparticles for MRI 5.1.1. MRI in General 5.1.2. Magnetic Nanoparticles as MRI Contrast AgentS 5.1.3. Cubic Ferrite Nanoparticles as T 2 -Weighted MRI Contrast Agents 5.1.4. Cubic Ferrite Nanoparticles as T 1 -Weighted MRI Contrast Agents 5.