Significance Al-MCM-41 catalyzed the three-component Strecker-type reaction of carbonyl compounds 1 , amines 2 , and TMSCN to afford the corresponding α-aminonitriles 3 in up to 100% yield (17 examples). Using Al-MCM-41 in a fixed-bed flow reactor, the desired α-aminonitrile 3a was constantly produced in nearly 80% yield for 48 h.