Black phosphorus (BP)-based two-dimensional (2D) nanomaterials are used as components in practical industrial applications in biomedicine, electronics, and photonics. There is a need to controllably shape engineered scalable structures of 2D BP building blocks, and their assemblyorganization is desired for the formation of three-dimensional (3D) forms such as macro and hybrid architectures, as it is expected that these architectures will deliver even better materials performance in applications.