The ability to shape and program remotely and contactlessly from two-dimensional (2D) flat multilayer materials into three-dimensional (3D) structures and functional devices could be ideal for applications like space missions, environmental remediation and minimally invasive surgery. However, achieving a fast and accurate deployment of complex 3D shapes contaclessly at low energy consumption, while embedding a number of physical properties and functionalities, remains very challenging. Herein, a strategy to widen the complexity space of 3D shapes and functions achievable is demonstrated, by enabling a controlled sequential folding while incorporating nano-reinforcements. Sequential folding was successfully achieved and a honeycomb structure was developed by designing multilayer polymer films with different kirigami patterns - each responding at a different rate upon heating. A finite element method (FEM) model was developed to better understand the main underlying physical mechanism as well as to feedback into materials and structure design. Moreover, a shape-programmed CNT veil-based honeycomb structure was developed, triggered remotely by thermal stimuli, with capability to self-sense the folding state through the electrical resistance change (ΔR/R0 = 100–300 %). Overall, it was demonstrated that designing layered nanocomposites with different 2D patterns allows an accurate sequential folding into 3D structures, with bespoke physical properties and integrated sensing–actuating functionalities.