An overview of the processing, characterization and magnetostructural properties of ferromagnetic NiMnX (X = group IIIA–VA elements) Heusler alloys is presented. This type of alloy is multiferroic—exhibits more than one ferroic property—and is hence multifunctional. Examples of how different synthesis procedures influence the magnetostructural characteristics of these alloys are shown. Significant microstructural factors, such as the crystal structure, atomic ordering, volume of unit cell, grain size and others, which have a bearing on the properties, have been reviewed. An overriding factor is the composition which, through its tuning, affects the martensitic and magnetic transitions, the transformation temperatures, microstructures and, consequently, the magnetostructural effects.