There has been a growing interest in two dimensional (2D) crystals beyond graphene, exhibiting novel properties and potential applications in next generation electronic and photonic devices. Graphene has superior properties, including high carrier mobility, ultrahigh surface area and excellent thermal conductivity. Whereas the lack of a band gap is a critical limitation for the use of graphene in electronic devices, monolayer semiconducting transition metal dichalcogenides (TMDs) have shown highly promising prospects in electronics and optoelectronics. Therefore, non-graphene 2D atomic layers, such as hexagonal boron nitride (hBN) and TMDs, have been integrated into research scale devices, thereby probing mechanical, chemical, electrical and optoelectrical functions. This abstract reports on our investigation of chemical vapour deposition (CVD)-growth, achieving localized, patterned, single crystalline or polycrystalline monolayers of TMDs, including MoS₂, WS₂, WSe₂ and MoSe₂, as well as their heterostructures. Particular focus is on enabling the fabrication of epitaxially grown TMDs on other van der Waals materials towards synthesizing TMDs with an ultralow-defect density. Furthermore the growth of TMD homobilayers with well-ordered stacking angles is demonstrated using the control of edge structures of the underlying TMD layer. Other nanomaterials, including vertically aligned carbon nanotubes for stretchable supercapacitors, are also investigated toward combining 2D materials with flexible substrates. Smart polymer functional surfaces using dodecylbenzenesulfonate-doped polypyrrole (PPy(DBS)) are also investigated to demonstrate in situ control of droplet pinning on the polymer surface, enabling the control of droplet adhesion from strongly pinned to extremely slippery (and vice versa). The pinning of organic droplets on the surfaces is dramatically controlled in situ, presenting great potential for manipulation and control of liquid droplets for various applications including oil separation, water treatment and anti-bacterial surfaces. We believe that our work represents a major advance in materials science and engineering, especially pertaining to those topics that involve functional and tunable surfaces.