In situ photocontrol over shear-thickening of condensed colloidal dispersions is of paramount importance in a wide range of applications including process technology and photorheological fluids. Its development and practicability, however, are hampered by the lack of well-designed photoresponsive systems. Here, a colloidal suspension whose rheological behavior is readily switchable between shear-thinning and shear-thickening using an external light stimulus is reported. This smart colloidal solution contains hybrid raspberry-like colloids prepared by employing cucurbit[8]uril as a supramolecular linker to assemble functional Fe3 O4 nanoparticles onto a silica core. The formed raspberry colloids are photoresponsive and can be reversibly disassembled under UV irradiation.