jats:pEven a century after the discovery of ferroelectricity, the quest for the novel multifunctionalities in ferroelectric and multiferroics continues unbounded. Vertically aligned nanocomposites (VANs) offer a new avenue toward improved (multi)functionality, both for fundamental understanding and for real-world applications. In these systems, vertical strain effects, interfaces, and defects serve as key driving forces to tune properties in very positive ways. In this Perspective, the twists and turns in the development of ferroelectric/multiferroics oxide–oxide and unconventional metal–oxide VANs are highlighted. In addition, the future trends and challenges to improve classic ferroelectric/multiferroic VANs are presented, with emphasis on the enhanced functionalities offered by existing VANs, as well as those in emerging systems.</jats:p>