Quantum dot superlattices, typically self-assembled on liquid-solid or liquid-liquid interfaces, have intrigued many for their unique electronic and optical properties. However, the fabrication process of these well-ordered structures is still limited by defect formations and control over allotropes. In this thesis, I delve into new self-assembly methods to achieve unique superlattice structures and a better understanding of quantum dot self-assembly by manipulating the self-assembly interface. Building upon past works on fundamental liquid-solid and liquid-liquid assemblies, I explore the prospect of using polymer brush films as an alternative substrate for quantum dot self-assembly, and to understand the interactions between quantum dots and polymer brushes. I will also explore self-assembled quantum dot colloidosomes through Pickering emulsion and investigate the molecular interactions for emulsion stabilization.