Manipulating cell-cell interactions is of great significance in cell communication and cell-based therapies. Although efforts have been made to construct cell-cell assembly by stimuli-responsive host-guest interactions, controllable cell-cell interactions by near-infrared (NIR) light triggered reversible assembly remain a challenge. Herein, we develop a NIR-controlled system based on β-cyclodextrin (β-CD) modified upconversion nanoparticles (UCNPs) for reversible and noninvasive manipulation of cell assembly and disassembly, which is realized by host-guest interactions between E/Z-photoisomerization of arylazopyrazole (AAP) and β-CD under the NIR irradiation. UCNPs can convert NIR to ultraviolet light, which leads to the transformation of AAP from the E-isomer to the Z-isomer. And it can be reverted back to the E-isomer under visible light irradiation. This reversible photoisomerization can modulate the host-guest interaction between β-CD and AAP, thus leading to reversible cell assembly and disassembly. Furthermore, by precise regulating cell-cell interactions by NIR light, cell-cell communication and molecular transportation can be realized. Given the diversity of host and guest molecules and the advantages of NIR light in biological applications, reversible cell-cell assembly has great potential for the regulation of cell behaviors and cell-based therapies.