To tailor the properties of colloidal materials, precise control over the self-assembly of their constituents is a prerequisite. Here, we govern the assembly of silica particles by functionalization with supramolecular moieties which interact with each other via directional and reversible hydrogen bonding. Through a generally applicable synthesis protocol, two different types of self-complementary hydrogen bonding moieties, BTA-and UPy-derivatives, are anchored to silica particles. Their selfassembly is initiated by the UV-induced removal of a photolabile protecting group, allowing the formation of hydrogen bonds between tethered molecules. The light-induced assembly of BTA-and UPy-decorated colloids in single-component dispersions and colloidal self-sorting in mixed dispersions is studied. Furthermore, we demonstrate that UPy-colloids can dissasemble upon addition of traces of a competitive binder (NaPy). This work provides further insight into the utility of supramolecular handles to orchestrate the assembly of micron-sized colloids via non-oligonucleotide hydrogen-bonding units.The ability to control molecular self-assembly via non-covalent interactions is an emerging bottom-up strategy to create complex metamaterials. In turn, well-defined molecular recognition can be used as a powerful tool to direct the assembly of micron-sized 1-3 colloids or even macroscopic objects 4 and create larger aggregated structures with emergent optical 5-7 , mechanical 8 or catalytic properties 9,10 . Molecular control over the assembly of micron-sized particles can be realized through particle surface-grafting of molecules exhibiting dipole-dipole 11,12 , metal coordination 13 , hydrophobic forces 14,15 and/or hydrogen bonding (H-bonding) [16][17][18] . Ideally, the tethered motifs should be easy to synthesize, responsive, externally addressable and provide directional, dynamic and specific bonding within the assemblies. Moreover, to facilitate colloidal assembly, a precise control between the interplay of non-specific surface forces (attractive and/or repulsive) is crucial 19 .A popular strategy in the field is the functionalization of colloids with complementary DNA strands 20,21 . Great advances in insight and structural complexity have been achieved in the last 20 years, enabling the assembly of colloids into both disordered and exotic ordered states 22,23 , in a reversible 22,24,25 or irreversible 26 manner and at the nano-27,28 and mesoscale 25,29 . Notwithstanding, DNA-technology has its limitations, such as high cost and restricted environmental conditions 27,30 because the strands only assemble in water at sufficiently high ionic strengths and at low temperature, precluding material synthesis and processing from organic solvents. Furthermore, up to now, only temperature has been used as external trigger of assembly, while recent advances towards light sensitive DNA-strands can be utilized in future to develop dual-responsive systems sensitive to both temperature and light 31 . A promising alternative strategy exploits...