Additionally, the packing of fullerenes onto substrates must be influenced by the shape and size, which would play a key role in the properties and stability of Phosphorene-Fullerene hybrids; then the physical/chemical phenomena that dominate the interaction strength is essential to be clarified. Mechanochemical reactions in a high energy mechanical milling process have been used as a strategy to form phosphorus-carbon (P-C) bonds between phosphorene and carbon materials, including C60, graphite, and graphite oxide ; in this way, the content of the P-C bond in the phosphorene-C60 hybrids is only 0.8%, denoting C60 is not preferably bonded to phosphorene via covalent interactions until breaking the sp 2 C=C/C-C bonds to form defects . In addition, low-temperature scanning tunneling microscopy, X-ray, ultraviolet photoelectron, and scanning tunneling spectroscopy measurements also show that C60 molecules are mainly physisorbed at room temperature on the honeycomb lattice of blue and black phosphorene synthesized by epitaxial growth, where an interfacial charge transfer is evidenced upon interaction with C60 .