Direct interaction with cultural heritage (CH) artefacts is frequently unavailable to visitors, offering an opportunity for HCI designers to explore integrating material aspects into digitally-mediated encounters with CH artefacts. We argue that a thorough understanding of the material experiences of CH artefacts can open a novel design space, enabling engaging and meaningful interactions with digital representations. Capitalising on this potential, we present a user study where we systematically explore the material experiences of historic pop-up and movable books. Our analysis identifies five key material qualities to inspire augmentation: fold-ability, slide-ability, tear-ability, age-ability, and print-ability. Highlighting how these material qualities can inspire novel interactions with their digital representations, we present two extended-reality (XR) prototypes of a CH book. With our work, we present HCI designers with a novel approach on designing CH experiences, firmly rooted in materiality, challenging the prevalent paradigms of 'technology-driven' or 'as-realistic-as-possible' sensory experiences often found in CH-HCI.