Supported ionic liquid-like phases (SILLPs) are able to efficiently catalyse the cyanosilylation of carbonyl compounds using trimethylsilyl cyanide under solvent-free conditions. These organic catalysts were efficient for various carbonyl compounds including aromatic, aliphatic and α,β-unsaturated. This process perfectly conforms to the features of green chemistry: no waste regarding side-products and unconverted reactants, solvent-free, excellent catalytic activity, and no requirement for separation. Furthermore the supported nature of the SILLPs allows for the development of continuous flow synthesis of cyanohydrin trimethylsilyl ethers. The effect of the morphology of the polymer (gel-type or macroporous bead resins or, alternatively, a monolithic polymer) has also been studied, which has allowed selecting suitable materials for the efficient continuous flow single pass synthesis of cyanohydrin trimethylsilyl ethers.