Two-dimensional layered materials (2DLMs) have received increasing attention for their potential in bioelectronics due to their favorable electrical, optical, and mechanical properties. The transformation of the planar structures of 2DLMs into complex 3D shapes is a key strategic step toward creating conformal biointerfaces with cells and applying them as scaffolds to simultaneously guide their growth to tissues and enable integrated bioelectronic monitoring. Using a strain-engineered self-foldable bilayer, we demonstrate the facile formation of predetermined 3D microstructures of 2DLMs with controllable curvatures, called microrolls. Three types of 2DLM microrolls─graphene, hexagonal boron nitride, and molybdenum disulfide─provide scaffolds to encapsulate and organize human-induced pluripotent stem cell-derived cardiomyocytes into tubular aggregates. Encapsulating cardiomyocytes in porous 2DLMs-laden microrolls allows for real-time microscopic observation and construction of precisely shaped cardiac tissues interacting with their surroundings. The ability to combine 2DLMs of diverse properties in the same structure further demonstrates the potential of this self-folding strategy for creating flexible, ultrathin bioelectronic devices that integrate seamlessly with complex biological environments, offering real-time, noninvasive monitoring of engineered tissues and organoids.